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33412 Publications

Effect of microbial siderophore DFOB on mobility and transport of Cu: Column experiment and reactive transport modelling

Karimzadeh, L.; Lippmann-Pipke, J.; Franke, K.; Lippold, H.; Fischer, C.
We focus on the transport behaviour of Cu under conditions related to a biohydrometallurgical leaching approach using neutrophilic microorganisms in neutral to slightly alkaline solutions. The effect of the microbial siderophore desferrioxamineB (DFOB) as a model leaching organic ligand on mobility and transport of Cu in the presence of kaolinite was investigated in column experiments. A geochemical transport model was established to describe the results. It was found that DFOB strongly enhances Cu mobility. The reactive transport model (including a surface complexation model) shows good agreement with the experimental data and is suitable to predict the transport behaviour of Cu in dependence on geochemical conditions.
The results of modeling revealed that in the absence of the ligand, a pH increase from 6.5 to 8.5 significantly retarded Cu breakthrough, whereas in the presence of DFOB, Cu breakthrough curves were nearly insensitive to pH changes and close to the breakthrough curve of a non-reactive tracer.
Keywords: Reactive transport modeling, Cu mobility, Microbial siderophore DFOB
  • Lecture (Conference)
    Computational Methods in Water Resources XXII (CMWR), 03.-07.06.2018, Saint Malo, France

Permalink: https://www.hzdr.de/publications/Publ-27313
Publ.-Id: 27313


In situ structural study of the surface complexation of lead(II) on the chemically mechanically polished hematite (1-102) surface

Qiu, C.; Majs, F.; Eng, P.; Stubbs, J.; Douglas, T.; Schmidt, M.; Trainor, T.
A structural study of the surface complexation of Pb(II) on the (View the MathML source) surface of hematite was undertaken using crystal truncation rod (CTR) X-ray diffraction measurements under in situ conditions. The sorbed Pb was found to form inner sphere (IS) complexes at two types of edge-sharing sites on the half layer termination of the hematite (View the MathML source) surface. The best fit model contains Pb in distorted trigonal pyramids with an average Pbsingle bondO bond length of 2.27(4) Å and two characteristic Pb-Fe distances of 3.19(1) Å and 3.59(1) Å. In addition, a site coverage model was developed to simulate coverage as a function of sorbate-sorbate distance. The simulation results suggest a plausible Pb-Pb distance of 5.42 Å, which is slightly larger than the diameter of Pb’s first hydration shell. This relates the best fit surface coverage of 0.59(4) Pb per unit cell at monolayer saturation to steric constraints as well as electrostatic repulsion imposed by the hydrated Pb complex. Based on the structural results we propose a stoichiometry of the surface complexation reaction of Pb(II) on the hematite (1-102) surface and use bond valence analysis to assign the protonation schemes of surface oxygens. Surface reaction stoichiometry suggests that the proton release in the course of surface complexation occurs from the Pb-bound surface O atoms at pH 5.5.
Keywords: Pb(II); Hematite; Crystal truncation rod

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Permalink: https://www.hzdr.de/publications/Publ-27312
Publ.-Id: 27312


Benchmark 3D reactive transport modelling of leaching of fractured calcareous sulfide ores

Karimzadeh, L.; Kulenkampff, J.; Schymura, S.; Lippmann-Pipke, J.
In the framework of the EU Horizon 2020 research project “BIOMOre” we developed a benchmark 3D reactive transport model to evaluate and predict insitu leaching (ISL) of fractured calcareous Kupferschiefer ore deposites. A critical challenge of our tasks is the implementation of the feedback between the evolution of porosity due to mineral dissolution/precipitation and modifications of the hydrodynamics of the reacting fluid. The sequential leaching of a calcareous sulfidic sandstone core (D=6 cm, L=10 cm) sampled from Kupferschiefer ore formation (Rudna mine, Poland) was done in laborytory. Here we present simulated results of the leaching of the core sample.
Geochemical modeling was performed by means of the COMSOL-PHREEQC interface iCP. The governing equations for fluid flow and conservative tracer transport are solved within the finite element code Comsol Multiphysics®. The geochemical processes considered in the model are kinetically controlled mineral dissolution and precipitation and equilibrium aqueous complexation reactions based on mass action law simulated by means of PHREEQC using BRGM database and advective-dispersive transport in the fracture and matrix diffusion in the rock mass calculated by COMSOL Multiphysics.
Calculated solution concentration of the outflow compares fairly well with the variation in the measured concentrations. Results showed that Cl is mainly released from halite which is totally removed in the washing stages. In addition our results showed that in stages 1, 2, and 3 about 0.04, 0.21, and 8.3% of Cu was extracted from sample respectively.
Keywords: reactive transport modeling, BIOMOre, insitu leaching
  • Lecture (Conference)
    Aachen International Mining Symposia (AIMS 2018), 23.-24.05.2018, Aachen, Germany

Permalink: https://www.hzdr.de/publications/Publ-27311
Publ.-Id: 27311


Advanced Analysis of Liquid Dispersion and Gas-Liquid Mass Transfer in a Bubble Column with Dense Vertical Internals

Möller, F.; Macisaac, A.; Lau, Y. M.; Schleicher, E.; Hampel, U.; Schubert, M.
The influence of dense vertical tube bundles in a batch bubble column reactor of 100 mm diameter and 1100 mm clear liquid height on liquid dispersion and gas-liquid mass transfer was studied. In particular, the effects of different tube patterns (triangular and square pitch), tube diameters (8 and 13 mm) and bottom end designs (flat and U-tube) having a tube diameter-to-pitch ratio of approx. 1.3 were investigated.
Dispersion coefficients were determined based on conductive tracer experiments recorded via wire-mesh sensors (WMS) with up to 90 measurement points distributed in the column’s cross-section in between the tubes. The gas-liquid mass transfer coefficient was determined via fast-responding oxygen needle probes. Tube pitch and pattern were identified as the most crucial design parameters for the extent of liquid dispersion. We found that particularly the U-tube bottom end design induces large liquid circulation patterns, which enhance dispersion. The presence of internals decreases the k_l a value as a consequence of turbulence damping, which is also confirmed by lower k_l values (e.g. 0.6 × 10-3 m s-1 for the empty BCR and 0.25 × 10-3 m s-1 for the square pitch with 8 mm tubes at 0.05 m s-1 superficial gas velocity), whereas the pitch is the most decisive design parameter. The U-tube bottom end design was identified as the most beneficial configuration with respect to liquid mixing and gas-liquid mass transfer.
Keywords: Bubble column, Heat exchanger internals, Gas-liquid mass transfer, 2D dispersion model, Wire-mesh sensor

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Permalink: https://www.hzdr.de/publications/Publ-27309
Publ.-Id: 27309


Evolution of the spin hall magnetoresistance in Cr2O3/Pt bilayers close to the Néel temperature

Schlitz, R.; Kosub, T.; Thomas, A.; Fabretti, S.; Nielsch, K.; Makarov, D.; Goennenwein, S. T. B.
We study the evolution of magnetoresistance with temperature in thin film bilayers consisting of platinum and antiferromagnet Cr2O3 with its easy axis out of the plane. We vary the temperature from 20 °C to 60 °C, in the vicinity of the Néel temperature of Cr2O3 of approximately 37 °C. The magnetoresistive response is recorded during rotations of the external magnetic field in three mutually orthogonal planes. A large magnetoresistance having a symmetry consistent with a positive spin Hall magnetoresistance is observed in the paramagnetic phase of Cr2O3, which however vanishes when cooling to below the Néel temperature. Compared to analogous experiments in a Gd3Ga5O12/Pt bilayer, we conclude that a paramagnetic moment in the insulator induced by an applied magnetic field is not sufficient to explain the observed magnetoresistance. We speculate that the type of magnetic moment at the interface qualitatively impacts the spin angular momentum transfer, with the 3d moments of Cr sinking angular momentum much more efficiently as compared to the more localized 4f moments of Gd.

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Permalink: https://www.hzdr.de/publications/Publ-27308
Publ.-Id: 27308


Competition of U(VI) hydroxide and carbonate complexation in alkaline solutions − implications for U(VI) retention by Ca-bentonite

Philipp, T.; Schmeide, K.; Rossberg, A.; Stumpf, T.
Thorough understanding of the aqueous complexation of U(VI) with ubiquitous inorganic ligands, such as hydroxide and carbonate, is crucial for predicting U(VI) mobility in natural and engineered systems, since retardation processes largely depend on the metal speciation. U(VI) hydrolysis [1] and complexation with carbonate in weakly alkaline media [2] have been extensively studied. This work systematically elucidates the U(VI) speciation in (hyper)alkaline solutions, where OH- and CO32- can occur in approximately equimolar quantities and compete for the complexation with U(VI). Such (hyper)alkaline conditions can evolve within deep geological repositories for radioactive waste by degradation of concrete. The effect of pH-dependent changes on the U(VI) sorption affinity was investigated by batch sorption experiments with Ca-bentonite, which is considered as buffer and backfill material within such repositories. Spectroscopic measurements provide information on the underlying retention mechanisms on the molecular level.
Time-resolved laser-induced fluorescence spectroscopy (TRLFS) proofs the formation of (calcium) uranyl carbonate complexes in aqueous solution in the presence of carbonate. However, these complexes only form up to a certain pH. A sudden change of the speciation to uranyl hydroxides was detected above pH 10 at low carbonate concentrations (0.5 mM) and above pH 11 at high carbonate concentrations (100 mM).
Batch sorption experiments reveal that this ligand replacement of carbonate by hydroxide correlates with an increase in U(VI) retention by Ca-bentonite. The study shows that an almost complete sorption of U(VI) can be obtained in (hyper)alkaline repository environments, even though carbonate is present in substantial amounts.
In order to clarify the mechanisms responsible for the very strong U(VI) retention, uranyl complexes on the bentonite surface were examined directly, using X-ray absorption spectroscopy (Rossendorf Beamline (ROBL), ESRF, Grenoble). Extended X-ray absorption fine structure (EXAFS) spectra did not show any indication of precipitates, implying that adsorption is the dominant retention process. In all samples with high U(VI) retention, the derived uranium coordination is identical irrespective of the amount of contained carbonate. According to atomic distances and coordination numbers, the U(VI) surface complexes shift from a 5-fold to a 4-fold coordination in the equatorial plane with increasing pH. Attachment might be facilitated by charge balancing cations (i.e. Ca2+) that mediate between the negatively charged clay surface and the anionic aqueous U(VI)-hydroxide complexes.
  • Poster
    18th Radiochemical Conference, 13.-18.05.2018, Marianske Lazne, Czech Republic

Permalink: https://www.hzdr.de/publications/Publ-27307
Publ.-Id: 27307


Charakterisierung der Bildqualität eines in-beam MR-Scanners an einer Protonenstrahlanlage während der Bestrahlung

Gantz, S.; Schellhammer, S. M.; Karsch, L.; Smeets, J.; Serra, A.; Pawelke, J.; Hoffmann, A. L.
Einleitung
Echtzeit-Magnetresonanztomographie kann die Präzision der Protonentherapie verbessern.
Ziel dieser Arbeit war die Charakterisierung der Bildqualität eines in-Beam MR-Scanners während der Bestrahlung.

Material & Methoden
Ein offener 0.22 T MR-Scanner (MrJ2200, Paramed) wurde im Isozentrum einer horizontalen Protonenstrahlanlage installiert. Die MR-Bildqualität wurde anhand zweier Komponenten beurteilt. Erstens wurde die Homogenität des Magnetfeldes des MR-Scanners innerhalb eines sphärischen Volumens von 22 cm Durchmesser mithilfe einer Magnetfeldkamera (MFC3045/48, Metrolab) vermessen. Dabei wurde der Einfluss der Strahlführungsmagnete, für Protonenenergien zwischen 70 und 220 MeV, untersucht. Zweitens wurde die Bildqualität ausgehend vom Protokoll des American College of Radiology (ACR) mittels des kleinen ACR Phantomes in einer dedizierten Kniespule untersucht. Hierzu wurden sowohl die vorgegebenen T1 und T2 Spin-Echo (SE) Sequenzen als auch zwei T1- und T2*-gewichtete Gradienten-Echo (GE) Sequenzen genutzt. Neben Referenzbildern mit ausgeschalteter Strahlanlage wurden Bilder in verschiedenen Szenarien sowohl unter dem Einfluss der Strahlführungsmagnete sowie unter direkter Bestrahlung aufgenommen. Hierfür wurde ein auf 10 mm Durchmesser kollimierter Strahl der Energie 125 MeV mit Dosisraten von 1 bzw. 80 Gy/min verwendet. ACR Bildparameter sowie Bildverschiebungen wurden mithilfe einer validierten Software (Matlab) ermittelt.

Ergebnisse
Die Magnetfeldhomogenität innerhalb des untersuchten Bereiches betrug 88 ppm (peak-to-peak). Unter dem Einfluss der Strahlführungsmagnete wurden Änderungen kleiner 3 ppm gemessen, weiterhin jedoch eine Verschiebung der mittleren Resonanzfrequenz, abhängig von der gewählten Strahlenergie, um 70 bis 110 Hz. Die T1-gewichteten GE Bilder enthalten Streifenartefakte; alle anderen SE und GE Bilder konnten ausgewertet werden. Es existieren keine signifikanten Unterschiede in den ACR Parametern zwischen den unterschiedlichen Szenarien. Bildverschiebungen in Frequenzkodierrichtung betrugen zwischen 0.5 und 3 mm und weisen eine indirekte Proportionalität zu den Gradientenstärken der einzelnen Sequenzen auf.

Zusammenfassung
Die Bildqualität des in-Beam MR-Scanners erfüllt die Spezifikationen des Herstellers sowie der ACR. Es wurde keine Änderung der MR-Bildqualität unter simultaner Bildgebung und Bestrahlung festgestellt, jedoch müssen Bildverschiebungen sequenzabhängig kompensiert werden.
  • Lecture (Conference)
    49. Jahrestagung der Deutschen Gesellschaft für Medizinische Physik, 19.-22.09.2018, Nürnberg, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-27306
Publ.-Id: 27306


Dual-Energy-Computertomographie ermöglicht Dosisberechnung auf Kontrastmittel-angereicherten CT-Aufnahmen

Möhler, C.ORC; Wohlfahrt, P.ORC; Greilich, S.ORC
Einleitung:
Falls bei der Therapieplanung CT-Kontrastmittel (KM) zur Diagnose und Konturierung eingesetzt wird, muss zur Dosisberechnung in der Regel ein weiteres, „natives“ CT-Bild ohne KM aufgenommen werden. Grund dafür ist der Einfluss der hohen Ordnungszahl des im KM enthaltenen Iods. Dieser kann durch den Einsatz von Dual-Energy-CT (DECT) korrigiert werden, was die Planung auf KM-angereicherten Bildern ermöglicht.

Material & Methoden:
Der Effekt eines gebräuchlichen KM (Imeron® 300, Bracco Imaging Deutschland GmbH) auf die ermittelte Elektronendichte wurde in CT-Bildern (a) einer Verdünnungsreihe in Wasser und (b) von 7 Hirntumorpatienten gemessen. Mit einem Somatom Definition Flash DECT-Scanner (Siemens Healthineers), ausgestattet mit zwei Röntgenröhren, wurden Bilder im 120 kVp Single-Energy-CT (SECT) Modus (nur a) und 80/140Sn kVp DECT-Modus (a und b) aufgenommen. Bei den Patienten (b) wurde jeweils ein Scan mit und ohne KM durchgeführt. Elektronendichte-Bilder wurden für SECT mit einer Hounsfield-Lookup-Tabelle und für DECT mit der Software Syngo.CT Rho/Z (Siemens Healthineers) erstellt.

Ergebnisse:
Bei der Verdünnungsreihe (a) führte der Einfluss des KM in den 120 kVp Bildern zu einer Überschätzung der Elektronendichte von 5-10% bei typischer Anreicherung (maximal 6 mg Iod/ml). Diese Verfälschung konnte durch den Einsatz von DECT auf unter 1% begrenzt werden. Bei den Patienten (b) betrug die mittlere Differenz zwischen den 120 kVp-äquivalenten Nativ- und KM-Bildern im Ganzhirn 1.5-4.4%, die entsprechende Differenz in den Elektronendichte-Bildern nur 0.2-0.6% (Abb. 1).

Zusammenfassung:
Der Einfluss von KM auf die Elektronendichte kann mittels DECT auf unter 1% reduziert werden. Dies ermöglicht den Verzicht auf einen zusätzlichen nativen Scan und somit eine Vereinfachung des klinischen Workflows und eine Reduktion der Strahlendosis auf die Hälfte.
Keywords: dual-energy CT, contrast agent, treatment planning, Kontrastmittel, Bestrahlungsplanung
  • Lecture (Conference)
    49. Jahrestagung der Deutschen Gesellschaft für Medizinische Physik, 19.-22.09.2018, Nürnberg, Deutschland

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Permalink: https://www.hzdr.de/publications/Publ-27305
Publ.-Id: 27305


Clinical feasibility of single-source dual-spiral 4D dual-energy computed tomography for proton treatment planning of lung-cancer patients

Wohlfahrt, P.ORC; Hofmann, C.; Troost, E. G. C.; Richter, C.; Jakobi, A.
Purpose/Objective:
Dual-spiral dual-energy CT (DECT) provides additional patient information to improve range accuracy in proton therapy, but is prone to motion between the two consecutively acquired scans. Here, the clinical feasibility of dual-spiral time-resolved DECT (4D-DECT) for proton treatment planning within the thoracic region was evaluated.

Material/Methods:
4D-DECT scans of three non-small-cell lung cancer (NSCLC) patients were acquired during the course of treatment with a Siemens single-source DECT scanner (Fig.1). For temporally averaged datasets and four breathing phases, the geometrical conformity of both 4D-DECT scans before (80kVp/140kVp) and after (58keV/79keV) image post-processing including deformable image registration (DIR) was assessed by normalized cross correlation (NCC).
To evaluate the reliability of dose calculation, clinical treatment plans were recalculated on DECT-derived 79keV MonoCT and 140kVp SECT datasets as reference using a heuristic conversion (HLUT) from CT number to stopping-power ratio (SPR). Dose distributions were compared with gamma analyses (0.1% dose-difference, 1mm distance-to-agreement criterion).
Finally, range differences between HLUT and patient-specific DECT-based SPR prediction were quantified.

Results:
Respiration changes during 4D-DECT acquisition resulted in NCCs>80%, indicating geometrical deviations of (1-2)mm. This was almost completely corrected by DIR leading to a high geometrical conformity with average NCC ± SD = (99.6±0.4)% corresponding to anatomical shifts below 0.2mm (not visually distinguishable). Even the impact of coughing could be corrected by DIR (Fig.2).
Clinical dose distributions on 140kVp and 79keV datasets were similar with average gamma passing rate of 99.9% and maximal dose difference of 0.8%.
Clinically relevant mean range shifts of (2.2±1.2)% were determined between patient-specific DECT-based SPR prediction and HLUT.

Conclusion:
Dual-spiral 4D-DECT is applicable for dose calculation on 79keV MonoCT datasets in NSCLC patients. Patient-specific DECT-based SPR prediction performed properly and revealed its potential for reducing range uncertainty. Even if large motion differences hamper 4D-DECT post-processing, only the 140kVp scan can be used and additional information on respiration variability and robustness is gathered.
Keywords: dual-energy CT, proton therapy, lung cancer, 4DCT, clinical feasibility
  • Lecture (Conference)
    49. Jahrestagung der Deutschen Gesellschaft für Medizinische Physik, 19.-22.09.2018, Nürnberg, Deutschland

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Permalink: https://www.hzdr.de/publications/Publ-27304
Publ.-Id: 27304


Clinical application of dual-energy CT for improved proton stopping-power prediction

Peters, N.; Wohlfahrt, P.; Möhler, C.; Enghardt, W.; Krause, M.; Troost, E.; Greilich, S.; Richter, C.
Purpose/Objective
The sub-percentage accuracy in proton stopping-power prediction of patient-individualized range prediction (PIRP) using dual-energy CT (DECT) was demonstrated in recent studies. Although DECT-derived pseudo-monoenergetic CT scans have been introduced into clinical routine, a heuristic conversion (HLUT) from CT number to stopping power ratio (SPR) is still necessary, Fig.1(1). We propose a method to refine the clinical HLUT by applying PIRP on a broad patient cohort as a step towards its clinical implementation.

Materials/Methods
Voxelwise correlations of CT number and SPR were obtained using DECT scans of 102 brain-tumor and 25 prostate-cancer patients treated with protons. The clinical HLUT was then refined by performing a step-wise weighted linear fit of the SPR distribution in different tissue regions, Fig.1(2). Furthermore, the intra- and inter-patient variability was quantified. To assess dose differences and range shifts, proton treatment plans were recalculated using the clinical and refined HLUT as well as PIRP.

Results
Between clinical HLUT and PIRP, mean range differences (±1SD) of (1.2±0.7)% for brain-cancer and (1.7±0.5)% for prostate-tumor patients were determined. On average, the clinical HLUT predicted larger SPR for brain, muscle and trabecular bone, leading to the systematic range deviations. They were significantly reduced (p≪0.001, two-sample t-test) below 0.3% by using the refined HLUT. However, an observed intra-patient soft-tissue diversity of 6% as well as an inter-patient bone diversity of 5% cannot be considered by any generic HLUT-based range prediction.

Conclusion
Retrospective application of PIRP allows for a reduction of systematic deviations found in clinical HLUT. In principal, this can also be transferred to particle-therapy centers not using DECT routinely. The refined HLUT was implemented at our institution as a step towards the currently ongoing full integration of PIRP. This includes the calibration, an end-to-end test as well as the quantification of prospects in safety margin reduction.
  • Lecture (Conference)
    49. Jahrestagung der Deutschen Gesellschaft für Medizinische Physik, 19.-22.09.2018, Nürnberg, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-27303
Publ.-Id: 27303


Organische Chemie XI - Chemie der Carbonylverbindungen

Mamat, C.
Nachdem wir uns sehr ausführlich über Verbindungen unterhalten haben, die Kohlenstoff-Kohlenstoff-Mehrfachbindungen enthalten (Alkene, Alkine, Aromaten), wollen wir zu Verbindungsklassen und funktionellen Gruppen kommen, bei denen Kohlenstoff-Heteroatom-Doppelbindungen existieren. Das sind insbesondere Aldehyde, Ketone, Carbonsäuren und deren Derivate. Im Gegensatz zu den nichtaktivierten C=C-Doppelbindungen sind diese Kohlenstoff-Heteroatom-Doppelbindungen bereits durch die Unterschiede in den EN-Werten aktiviert. Wir finden ein elektronegatives Zentrum am Heteroatom (Sauerstoff, Stickstoff oder Schwefel) und ein elektropositives Zentrum am Kohlenstoff. Somit ist die Regioselektivität bei nucleophilen bzw. elektrophilen Angriffen vorgegeben. Wenn beispielsweise Nucleophile an diese Doppelbindung angreifen, werden sie spezifisch an den Kohlenstoff gebunden, wohingegen die Elektrophile den Sauerstoff angreifen. Neben der Carbonylgruppe, in der der Sauerstoff über eine Doppelbindung gebunden ist gibt es auch carbonylanaloge Verbindungen mit Stickstoff oder Schwefel, wobei die Elektronegativitätsdifferenz und damit die Polarisierung der Doppelbindung in der Richtung O > N > S abnimmt.
  • Book (Authorship)
    Heidelberg: Springer Verlag, 2018
    0049 Seiten

Permalink: https://www.hzdr.de/publications/Publ-27302
Publ.-Id: 27302


Organische Chemie X - Aromatische Substitution

Mamat, C.
In den vergangenen Heften haben wir uns ausführlich über die Reaktionen an gesättigten und ungesättigten Kohlenstoffatomen unterhalten, wobei wir die aromatischen Vertreter geflissentlich ausgelassen haben. Außerdem haben wir geschaut, welche Effekte diese Aromaten bzw. aromatische Reste wie Phenylgruppen auf die Stabilität von Zwischenstufen wie Carbanionen, Carbokationen oder Radikalen ausüben und welche Konsequenzen sich aus diesem Einfluss dann auf die Reaktivität und /oder (Regio-)Selektivität der Derivate ergeben.
  • Book (Authorship)
    Heidelberg: Springer Verlag, 2018
    0035 Seiten

Permalink: https://www.hzdr.de/publications/Publ-27301
Publ.-Id: 27301


Organische Chemie IX - Additionsreaktionen

Mamat, C.
Additionen sind die mit Abstand wichtigsten Reaktionen von ungesättigten Verbindungen (Alkenen, Alkinen, aber auch Carbonylverbindungen). Formal handelt es sich dabei um die Umkehrung der Eliminierungsreaktionen. Additionsreaktionen können radikalisch oder ionisch verlaufen. Im Falle eines ionischen Verlaufs können wir noch zwischen einem elektrophilen oder einem nucleophilen ersten Angriff auf die Doppelbindung unterschieden. Der vierte Typ umfasst die große Gruppe der Cycloadditionen. Diese pericyclischen Reaktionen kommen ohne geladene Teilchen aus und verlaufen meist konzertiert. Somit sind vier Typen von Additionen an die Doppelbindung zu unterscheiden.
  • Book (Authorship)
    Heidelberg: Springer Verlag, 2018
    0051 Seiten

Permalink: https://www.hzdr.de/publications/Publ-27300
Publ.-Id: 27300


Organische Chemie VIII - Eliminierungsreaktionen

Mamat, C.
Wir haben schon aus den Studienheften der Organischen Chemie I erfahren, dass Eliminierungsreaktionen am sp3- oder sp2-hybridisierten Kohlenstoff die Umkehrung von Additionsreaktionen sind. Sie treten damit als Konkurrenzreaktion zu den nucleophilen Substitutionen auf und führen generell zu ungesättigten Verbindungen (Alkenen oder Alkinen). Dabei müssen zwei σ-Bindungen gebrochen werden. Aus den beteiligten sp3-hybridisierten Kohlenstoffatomen werden sp2-hybridisierte gebildet und als Konsequenz daraus bilden sich nach Abspaltung aus sp2-hybridisierten Kohlenstoffatomen sp-hybridisierte, die an der jeweiligen Mehrfachbindung beteiligt sind. Neben der σ-Bindung zwischen den beteiligten Kohlenstoffatomen wird nun eine oder zwei π-Bindungen ausgebildet. Dabei entstehen kleine, stabile Moleküle wie z. B. Halogenwasserstoff (HCl, HBr), Wasser, CO2 und andere als eliminierte Nebenprodukte.
  • Book (Authorship)
    Heidelberg: Springer Verlag, 2018
    0030 Seiten

Permalink: https://www.hzdr.de/publications/Publ-27299
Publ.-Id: 27299


Organische Chemie VII - Radikalische und nucleophile aliphatische Substitution

Mamat, C.
Nachdem wir uns ausführlich mit den wichtigsten Stoffklassen und funktionellen Gruppen in der organischen Chemie beschäftigt haben, wollen wir nun im zweiten Teil noch einmal auf die Reaktionen und ihre Mechanismen schauen. Diese Mechanismen sind wichtige Werkzeuge, um zu verstehen, warum Reaktionen funktionieren oder auch nicht. Oder warum das eine Produkt gebildet wird und das andere nicht. Oftmals haben wir auch Konkurrenzsituationen, wie die Eliminierung bei der nucleophilen Substitution oder auch zwei (oder mehrere) reaktive Zentren, an denen die Reaktion prinzipiell ablaufen könnte. In solchen Situationen werden wir sehen, dass eine Steuerung möglich ist, je nachdem wie die Reaktionsbedingungen gewählt werden. Ein weiterer wichtiger Faktor wird durch die Kinetik der Reaktionen beschrieben. Sie gibt ebenfalls Auskunft darüber, ob und wie Reaktionen ablaufen. Wenn das alles nicht hilft, gibt es die Möglichkeit, funktionelle Gruppen, die nicht reagieren sollen, mit Schutzgruppen vor der Reaktion zu blockieren. Damit wird ebenfalls eine regioselektive Reaktion erreicht.
  • Book (Authorship)
    Heidelberg: Springer Verlag, 2018
    0040 Seiten

Permalink: https://www.hzdr.de/publications/Publ-27298
Publ.-Id: 27298


Assessment of RBE variability in proton therapy using a Monte-Carlo method

Eulitz, J.; Dutz, A.; Lutz, B.; Wüstemann, J.; Wohlfahrt, P.; Oesten, H.; Hahn, C.; Permatasari, F.; Löck, S.; Krause, M.; Enghardt, W.; Troost, E. G. C.; Lühr, A.
Introduction
Routinely, a constant relative biological effectiveness (RBE) is used in proton therapy. However, experimental evidence indicates that RBE can vary with dose and linear energy transfer (LET). Here, we introduce a Monte-Carlo simulation method to assess RBE variations from follow-up magnetic resonance (MR) scans and illustrate its applicability for an exemplary brain-tumor patient.
Methods
A proton therapy Monte-Carlo model was setup to simulate dose and dose-averaged LET distributions of treatment fields on computed tomography (CT) scans and also in a water phantom for comparison with quality assurance measurements. A follow-up T1-weighted contrast-enhanced (T1w-CE) MR scan of an astrocytoma (grade 2) patient, acquired 18 months after radiochemotherapy (DRBE=1.1=60Gy), was used to delineate post-treatment image-change regions and rigidly co-registered to the planning CT. A multivariable logistic normal tissue complication model (NTCP) was built by voxel-wise correlating image changes with simulated dose and LET distributions. Tolerance doses TD10 (resulting in 10% probability of image change in a voxel) as function of LET were obtained from the NTCP model.
Results
Measured and Monte-Carlo-predicted dose agreed within 2%. Changes on follow-up T1w-CE-MR images correlated with increasing simulated dose and LET (Fig.1). The NTCP model revealed a significant LET effect (p<0.0001) on the image change probability resulting in a decrease of modeled TD10 values from 70.3Gy to 50.6Gy for 1keV/μm and 6keV/μm, respectively, indicating a varying RBE (Fig.2).
Conclusion
The correlation of post-treatment MR image changes with Monte-Carlo simulations allows for testing the hypothesis of a variable proton RBE. Currently, this method is systematically evaluated and may, after validation in independent patient cohorts, reduce biological uncertainty in proton therapy.
  • Lecture (Conference)
    49. Jahrestagung der Deutschen Gesellschaft für Medizinische Physik, 19.-22.09.2018, Nürnberg, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-27296
Publ.-Id: 27296


Charge Carrier Dynamic in Ga1-xMnxAs Studied by Resistance Noise Spectroscopy

Lonsky, M.; Teschabai–Oglu, J.; Pierz, K.; Sievers, S.; Schumacher, H. W.; Yuan, Y.; Böttger, R.; Zhou, S.; Müller, J.
We report on electronic transport measurements of the magnetic semiconductor Ga1-xMnxAs, whereby the defect landscape in various metallic thin films (x = 6%) was tuned by He-ion irradiation. Changes in the distribution of activation energies, which strongly determine the low-frequency 1/f-type resistance noise characteristics, were observed after irradiation and can be explained by deep-level traps residing in the As sublattice. Various other kinds of crystalline defects such as, for instance, Mn interstitials, which possibly form nanoscale magnetic clusters with a fluctuating spin orientation, also contribute to the 1/f noise and can give rise to random telegraph signals, which were observed in films with x = 7%. In addition, we neither find evidence for a magnetic polaron percolation nor any features in the noise near the Curie temperature.

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Publ.-Id: 27295


Absolute Hugoniot measurements from a spherically-convergent shock using x-ray radiography

Swift, D. C.; Kritcher, A.; Hawreliak, J.; Lazicki, A.; Macphee, A.; Bachmann, B.; Döppner, T.; Nilsen, J.; Collins, G. W.; Glenzer, S.; Rothman, S. D.; Kraus, D.; Falcone, R. W.
The canonical high pressure equation of state measurement is to induce a shock wave in the sample material and measure two mechanical properties of the shocked material or shock wave. For accurate measurements, the experiment is normally designed to generate a planar shock which is as steady as possible in space and time, and a single state is measured. A converging shock strengthens as it propagates, so a range of shock pressures is induced in a single experiment. However, equation of state measurements must then account for spatial and temporal gradients. We have used x-ray radiography of spherically-converging shocks to determine states along the shock Hugoniot. The radius-time history of the shock, and thus its speed, was measured by radiographing the position of the shock front as a function of time using an x-ray streak camera. The density profile of the shock was then inferred from the x-ray transmission at each instant of time. Simultaneous measurement of the density at the shock front and the shock speed determines an absolute mechanical Hugoniot state. The density profile was reconstructed using the known, unshocked density which strongly constrains the density jump at the shock front. The radiographic configuration and streak camera behavior were treated in detail to reduce systematic errors. Measurements were performed on the Omega and National Ignition Facility lasers, using a hohlraum to induce a spatially uniform drive over the outside of a solid, spherical sample, and a laser-heated thermal plasma as an x-ray source for radiography. Absolute shock Hugoniot measurements were demonstrated for carboncontaining samples of different composition and initial density, up to temperatures at which K-shell ionization reduced the opacity behind the shock. Here we present the experimental method, using measurements of polystyrene as an example.

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Publ.-Id: 27294


Using time-resolved penumbral imaging to measure low x-ray emission signals from capsule implosions at the NIF

Bishel, D. T.; Bachmann, B.; Yi, A.; Kraus, D.; Divol, L.; Falcone, R. W.; Fletcher, L. B.; Glenzer, S. H.; Landen, O. L.; Macdonald, M. J.; Masters, N.; Neumayer, P.; Redmer, R.; Saunders, A. M.; Witte, B.; Döoppner, T.
We have developed an experimental platform at the National Ignition Facility to measure x-ray Thomson scattering (XRTS) spectra from indirectly-driven capsule implosions that create extreme density conditions near stagnation [D. Kraus et al, J. Phys. Conf. Series 717, 012067 (2016).]. In order to account for shot-to-shot variations of the stagnation time and to benchmark the achieved plasma conditions between shots and against radiation hydrodynamics simulations, we need to know the relative timing between the scattering measurement and the peak x-ray emission, which occurs at stagnation. Due to lower implosion velocity, use of a low gas fill capsule, and hot spot symmetry perturbations, the hot spot emission is 100 - 1000x weaker than that of standard ICF implosions. To address this challenge, we have developed and fielded a new pinhole-imaging snout that exploits time-resolved penumbral imaging. Using 150 µm diameter penumbral-imaging pinholes, a time series of 2D images can be reconstructed through analysis of the penumbras. The reconstructions allow us to extract the spatially and temporally resolved evolution and timing of the implosion through stagnation. We use differential filtering to extract plasma temperatures, additionally constraining the thermophysical plasma conditions. Despite fluctuations of the x-ray flash intensity of up to 5x, the emission time history is similar from shot to shot, and slightly asymmetric with respect to peak x-ray emission. Peak emission times vary by up to 250 ps and can be determined with an accuracy of 50 ps.

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Publ.-Id: 27293


Hybrid plasma wakefield acceleration: Concept & preliminary results

Kurz, T.ORC; Heinemann, T.; Knetsch, A.; Couperus, J. P.; Köhler, A.; Zarini, O.; Hidding, B.; Assmann, R.; Bussmann, M.; Osterhoff, J.; Schramm, U.; Martinez De La Ossa, A.; Irman, A.
Plasma wakefield accelerators can be driven by either a powerful laser pulse (LWFA) or a high-current charged particle beam (PWFA). We combine both acceleration methods in a staged setup to efficiently exploit the advantages of each scheme. We present preliminary results of a proof of concept-experiment at the DRACO laser facility at Helmholtz-Zentrum Dresden-Rossendorf (HZDR). The LWFA stage (1st stage) generates ultra relativistic electron beams with peak currents exceeding 20kA via self truncated inonization injection (STII) out of a 3mm super sonic dopant (He+N) gas jet. These beams are sent into the second 3mm dopant (H+He) gas jet, driving plasma wakefields in the non-linear bubble regime. Thereby, injected electrons induced by the field ionization form a second electron beam (witness) that ideally exeeds the driving bunch (driver) quality in terms of energy and brightness.
  • Lecture (Conference)
    DPG - Frühjahrstagung, 19.-23.03.2018, Würzburg, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-27292
Publ.-Id: 27292


Calibration and cross-laboratory implementation of scintillating screens for electron bunch charge determination

Kurz, T.ORC; Couperus, J. P.ORC; Krämer, J. M.ORC; Ding, H.; Kuschel, S.; Köhler, A.; Zarini, O.; Hollatz, D.; Schinkel, D.; D'Arcy, R.; Schwinkendorf, J. P.; Irman, A.ORC; Schramm, U.ORC; Karsch, S.
In this article we revise the calibration measurements of different scintillation screens commonly used for the detection of relativistic electrons, extending previous reference work towards higher charge density and new types of screens. Electron peak charge densities up to 10 nC/mm² were provided by focused picosecond-long electron beams delivered by the ELBE linear accelerator at the Helmholtz-Zentrum Dresden-Rossendorf.
At low charge densities, a linear scintillation response was found, followed by the onset of saturation in the range of nC/mm². The absolute calibration factor (photons/sr/pC) in this linear regime was measured to be almost a factor of 2 lower than reported by Buck et al. retrospectively implying a higher charge in charge measurements performed with the old calibration. A good agreement was found with the results by Glinec et al.. Furthermore long-term irradiation tests with an integrated dose of approximately 50 nC/mm² indicate a significant decrease of the scintillation efficiency over time.
Finally, in order to enable the transfer of the absolute calibration between laboratories, a new constant reference has been developed.

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Publ.-Id: 27291


Interdisciplinary round-robin test on molecular spectroscopy of the U(VI) acetate system

Müller, K.; Foerstendorf, H.; Steudtner, R.; Tsushima, S.; Kumke, M. U.; Lefèvre, G.; Rothe, J.; Mason, H.; Szabó, Z.; Yang, P.; Adam, C.; André, R.; Brennenstuhl, K.; Cho, H.; Creff, G.; Coppin, F.; Dardenne, K.; Den Auwer, C.; Drobot, B.; Eidner, S.; Hess, N. J.; Kaden, P.; Kremleva, A.; Kretzschmar, J.; Krüger, S.; Platts, J. A.; Panak, P. J.; Polly, R.; Powell, B. A.; Rabung, T.; Redon, R.; Reiller, P. E.; Rösch, N.; Rossberg, A.; Scheinost, A. C.; Schimmelpfennig, B.; Schreckenbach, G.; Skerencak-Frech, A.; Sladkov, V.; Solari, P. L.; Wang, Z.; Washton, N. M.; Zhang, X.
In the advent of the 2nd International Workshop on Advanced Techniques in Actinide Spectroscopy (ATAS 2014), an inter-laboratory round-robin test (RRT) was initiated. The main goal of this RRT was the comprehensive molecular analysis of a simple aqueous com-plexing system – U(VI) acetate – which was selected to be independently investigated by various spectroscopic (vibrational, luminescence, X-ray absorption, and nuclear magnetic resonance spectroscopy) and quantum chemical methods applied by leading laboratories in actinide or geochemical research. Ultimately, more than 40 scientists hosted at twenty insti-tutions in seven countries participated.
The outcome of this RRT can be considered on two levels: First, conformities as well as discrepancies in the results of each spectroscopic technique and their sources are evaluated. The raw data from the experimental approaches were found to be generally consistent. In particular, for complex setups such as accelerator-based X-ray absorption spectroscopy, the agreement between the raw data was surprisingly high. By contrast, the data obtained using luminescence spectroscopy turned out to be strongly related to the chosen acquisition pa-rameters. Second, the potentials and limitations of coupling various spectroscopic and, in particular, theoretical approaches for the comprehensive study of actinide molecule com-plexes are assessed. The additional benefits of the combined approach with regard to the exploration of the aqueous speciation of the U(VI) acetate system are elaborated.
Keywords: Uranium, acetic acid, actinides, spectroscopy, infrared, Raman, vibrational, luminescence, fluorescence, magnetic resonance, X-ray absorption, Quantum chemistry, ATR FT-IR, TRLFS, NMR, EXAFS, density functional theory, DFT, wave function theory, MP2

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Publ.-Id: 27289


Production and Characterization of the 163Ho Source for the ECHo Project

Wendt, K.; Düllmann, C. E.; Kieck, T.; Dorrer, H.; Mokry, C.; Rugel, G.; Wiescher, F.; Merchel, S.ORC; Forstner, O.
The ECHo (Electron Capture in Holmium Experiment) collaboration aims at measuring the electron neutrino mass by recording the spectrum following electron capture of 163Ho using metallic magnetic calorimeters. The radioisotope 163Ho (t1/2 = 4570 a) is produced by neutron capture from enriched 162Er in the Institute Laue-Langevin high-flux nuclear reactor. After chemical separation the important step of embedding the sample into the 180x180 𝜇m2 Au-absorbers of the ECHo detectors is carried out by laser mass spectrometric techniques. The application of multi-step resonance ionization at the 60 kV RISIKO mass separator of Mainz University ensures highest efficiency and unrivalled elemental and isotopic selectivity for ultra-pure 163Ho ion implantation with sub-millimeter beam spot. The efficiency and stability of the laser ion source and the implantation process is permanently monitored and improved to minimize any losses of the precious sample material, while an in-situ deposition of gold by parallel pulsed laser deposition (PLD) ensures a homogeneous 163Ho/Au layer production and prevents disturbing sputter effects. To screen the purity of the source from production up to use besides a number of more conventional analytical techniques accelerator mass spectrometry (AMS) of Ho at the AMS-facility of the Helmholtz-Zentrum Dresden-Rossendorf is under development to address the very low content in the 10 or lower region of the radiocontaminating isotope 166mHo (t1/2 = 1200 a).
Keywords: AMS, Holmium, electron capture, mass separator
  • Lecture (Conference)
    Workshop on Ion and Particle Beams (Ionenstrahl Workshop), 24.-25.03.2018, Darmstadt, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-27288
Publ.-Id: 27288


High Speed, High Resolution Imaging Spectrometers Based on pnCCDs for XRF and XRD Applications

Strüder, L.; Hartmann, R.; Holl, P.; Ihle, S.; Huth, M.; Schmidt, J.; Thamm, C.; Kanngießer, B.; Baumann, J.; Renno, A. D.ORC; Grenzer, J.; Radtke, M.; Abhoud, A.; Pietsch, U.; Soltau, H.
For many years pnCCDs have been well known as X-ray detectors for spectroscopic imaging in many fields of science: X-Ray Fluorescence analysis (XRF), X-ray Diffraction (XRD) with light sources in large accelerator facilities as well as with laboratory light sources or with X -rays from celestial sources in X-ray astronomy. A brief introduction in GEXRF (Grazing Emission XRF) measurements with a laboratory laser produced plasma source will be given, PIXE (Particle Induced X-ray Emission) measurements and D2XRF (Double Dispersive X -Ray Fluorescence) and Slicing experiments with pnCCDs coupled to polycapillary optics performed at the BESSY synchrotron will be shown. Energy - dispersive Laue diffraction with ultra - hard X-rays for the analysis of defects in metals will conclude the overview of spectroscopic X-ray imaging measurements in the field of structure and dynamics of matter. pnCCDs are radiation detectors on high resistivity 450 μm thick fully sensitive silicon [1]. They are back-illuminated devices with an ultra-thin, homogeneous radiation entrance window, enabling the proper detection of X-rays up to 30 keV with high quantum efficiency. As all pnCCDs are equipped with a fully column parallel readout, frame rates on more than 1200 frames per second are achieved, keeping the read noise level at 3 electrons (rms). Some of the key performance figures are (1) a quantum efficiency above 90% from 1 keV up to 10 keV, (2) single photon counting capability starting at only 30 eV, (3) extreme radiation hardness due to the avoidance of active MOS structures, and (4) energy resolution of 130eV (FWHM) at 6 keV and 37 eV (FWHM) at 90 eV. These properties have enabled a variety of spectacular measurements. (a) GEXRF: By combining a highly brilliant laser produced plasma (LPP) source with a scanning - free setup, grazing emission X-ray fluorescence (GEXRF) measurements in the soft X - ray range were realized [2]. The detector, a pnCCD, was operated in a single photon counting mode in order to utilize its energy dispersive properties. GEXRF profiles of the Ni - Lα line of a carbon - nickel multilayer sample, which displays a lateral (bi-)layer thickness gradient, were recorded at several positions. Simulations of theoretical profiles predicted a prominent intensity dip at emission angles between 5° and 12°, depending strongly on the bi-layer thickness of the sample (see Fig.1). This information was used to retrieve the bi - layer thickness gradient. The results are in good agreement with values obtained by X-ray reflectometry, conventional X-ray fluorescence and transmission electron microscopy measurements and serve as proof of principle for the suggested GEXRF setup. (b) PIXE: The unique properties pnCCDs, coupled to polycapillary X-ray optics, allows a fast position resolved overview over a large detection area with first results visible in real time. The maximum field of view exceeds 1 cm2 and the spatial resolution approaches a few microns when using sub-pixel algorithms by centroiding the signal charge cloud in the pixel structure [3] .
The device has been used as an X-ray detector at the PIXE beamline at the Helmholtz-Zentrum Dresden Rossendorf (see Fig. 2). In addition to the above measurements (c) D2XRF and Slicing experiments performed at the BESSY synchrotron will be presented (see Fig. 3) as well as (d) Energy Dispersive Hard X-ray Laue Diffraction measurements at the ESRF.
Keywords: pnCCD, High-Speed PIXE
  • Contribution to proceedings
    Microscopy and Microanalysis 2016, 24.07.2016, Columbus, USA
    Proceedings of Microscopy and Microanalysis 2016, 100-101
    DOI: 10.1017/S1431927616001355

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Publ.-Id: 27286


Neptunium(V) transport in granitic rock: A laboratory scale study on the influence of bentonite colloids

Elo, O.; Hölttä, P.; Kekäläinen, P.; Voutilainen, M.; Huittinen, N.
In the present study neptunium(V) uptake by crystalline granitic rock (Kuru Grey granite) and bentonite colloids (MX-80) under stagnant conditions in batch-type experiments and the role of stable and mobile bentonite colloids on the migration of neptunium(V) through intact granite columns under flowing water conditions was investigated. The uptake of 10-6 M neptunium(V) by 40 g/L crushed granite in 10 mM NaClO4 was found to be pH-dependent, whereas neptunium(V) uptake by MX-80 bentonite colloids (0.08-0.8 g/L) was pH-independent up to a pH-value of approximately 11. Column experiments were conducted in the presence and absence of colloids at two pH values (pH = 8 and 10) and two flow rates (0.3 mL/h and 0.8 mL/h) in 10 mM NaClO4. The neptunium(V) concentration was 2×10-4 M and the colloid concentration ranged from 0.1-1 g/L. The properties of the flow field in the columns were investigated with a conservative chloride tracer, at the same two flow rates of 0.8 and 0.3 mL/h. The resulting breakthrough curves were modeled using the analytical solution of advection–matrix diffusion equation. Based on the column experiments, neptunium(V) association with the colloids was found to occur directly in the injection phase. At slow flow rate, no influence of the bentonite colloids could be seen, implying that the non-sorbed and colloid-borne neptunium(V) are eluted from the columns at pH = 8 and that an exchange from colloid-borne to granite-sorbed neptunium(V) occurred at pH = 10. For the higher flow rate at pH = 8, clogging of flow channels, resulting in an enhanced retention of colloid-associated neptunium(V) was found. At pH = 10, adsorption of neptunium(V) on the granite reduced the clogging effect.
Keywords: Neptunium(V), Bentonite colloids, Granitic rock, Sorption, Column experiments

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Publ.-Id: 27285


Model-driven parameter reconstructions from Small Angle X-ray Scattering images

Zacharias, M.
The diagnostic of plasma dynamical processes at solid densities and at the time and length scales involved in the formation of instabilities has become accessible in experiments by coherent X-ray scattering techniques through the advent of X-ray free-electron lasers. In this thesis, models for the density of structured targets under the influence of plasma expansion are studied. A general analytical derivation of the scattering signal of such targets is given and it is investigated what kind of statements regarding the expansion profile can be made based on data analyses that comprise various parametrical density models. To enable numerical investigations of experimental X-ray intensities with reduced parametrical density models, a framework has been designed in Python. The operability of the framework is demonstrated with data from experiments. Based on the results, statistically robust multi-model reconstructions of the plasma density that use the presented framework are envisioned.
Keywords: SAXS, small angle X-ray scattering, XFEL, reconstruction, plasma, numerical, Python
  • Master thesis
    TU Dresden, 2017
    Mentor: Dr. Thomas Kluge, Dr. Michael Bussmann, Prof. Dr. Ulrich Schramm, Prof. Dr. Thomas E. Cowan
    0090 Seiten
    DOI: 10.5281/zenodo.1208410

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Publ.-Id: 27284


Ultrafast response of photoexcited carriers in VO₂ at high-pressure

Braun, J. M.; Schneider, H.; Helm, M.; Mirek, R.; Boatner, L. A.ORC; Marvel, R. E.; Haglund Jr., R. F.; Pashkin, A.ORC
We utilize near-infrared pump — mid-infrared probe spectroscopy to investigate the ultrafast electronic response of pressurized VO₂. A clear anomaly in the linear mid-infrared response as well as in the fluence dependence of the pump-probe signal is observed around 8 GPa indicating a pressure-induced phase transition. Distinct pump-probe signals and a pumping threshold behavior typical for the insulating VO₂ phase persist also in the high-pressure phase. Thus, in contrast to the temperature-induced rutile metallic state of VO₂, the pressure-induced monoclinic phase preserves the energy gap. However, our results indicate the appearance and a gradual growth of additional intragap states upon increasing pressure above 8 GPa. These observations can be interpreted in terms of a bandwidth-controlled Mott – Hubbard transition.
Keywords: metal-insulator transition, vanadium dioxide, ultrafast spectroscopy, high-pressure
Related publications
Ultrafast carrier dynamics in VO₂ across the … (Id 25953) is previous version of this publication

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Development of an efficient high-current ion source for Accelerator Mass Spectrometry

Hofsäss, H.; Bregolin, F.; Yordanov, D.; Rugel, G.; Akhmadaliev, S.; Merchel, S.ORC; Feige, J.
A new efficient negative ion source for Accelerator Mass Spectrometry (AMS) is being built to quantify the ratios of long-lived cosmogenic radionuclides in micrometeorites. Measuring these extremely small ratios is at the technological limits of present AMS systems. The new source is designed specifically to provide a higher AMS detection sensitivity by having an optimal ion-optics design, incorporating new concepts for the construction and operation of the Cs ionizer, optimized Cs ion beam currents and Cs vapor transport, as well as the operation with higher cathode voltages than usual. Moreover, its design is modular providing ease of access and simplifying maintenance while providing better mechanical stability. Several source parameters can be controlled and measured during operation to achieve a better source performance. The new source will consist of a auto-aligning modular ionizer, a Cesium supply with active temperature control of the supply tubes, a novel shroud for the Cs supply and a cathode operated at up to -20 kV cathode bias. The design is optimized using COMSOL ion optics simulations, including space charge effects, thermal transport simulations as well as detailed sputter simulations. The authors would like to thank the Federal Ministry of Education and Research of Germany for its financial support (project 05K2016), and the HZDR's Ion Beam Center for its essential contribution to the realization of this project.
Keywords: AMS, micrometeorite
  • Lecture (Conference)
    Workshop on Ion and Particle Beams (Ionenstrahl Workshop), 24.-25.03.2018, Darmstadt, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-27282
Publ.-Id: 27282


Homogeneous pressed powder pellets as new MRMs for in situ microanalytical techniques

Garbe-Schönberg, D.; Müller, S.; Nordstad, S.; Wiedenbeck, M.; Renno, A. D.ORC
While in-situ analytical instrumentation for the direct elemental and isotopic analysis of solid materials has undergone continuous and significant improvement over recent years, development of well-characterized and homogeneous microanalytical reference materials (MRM) for calibration and validation of analytical data has been delayed. Ideally, MRM must be homogeneous down to the single micrometer scale for major, minor, trace, and ultra-trace elements and isotopes, withstand high-vacuum and impact of high-energy electron, ion, and photon beams, stable in its physical and chemical properties over time and under various environmental conditions, certified following ISO guidelines, and available for a wide variety of materials.
We developed a method for manufacturing undiluted, binder-free pressed powder pellets[1] with particle grain size down to the nanometer range (D50 <170 nm), extremely low roughness of pellet surface (RA <50 nm), and excellent within and between pellet homogeneity. This technique has been applied so far to a wide range of very different sample types: biogenic carbonates (foraminifera, clam shells, red algae, corals), speleothem, silicate rocks, iron ores and banded iron formation, manganese nodules, sulphides UQAC-FeS, refractory minerals, plutonic and volcanic rocks, fly ash, bone-apatite, minerals for Rb/Sr age-dating[2] etc.. We successfully blended different materials opening new ways for producing e.g., series of elemental and isotopic calibration standards. These “nanopellets” have been successfully used with LA-ICP-MS, LIBS, µ-XRF, handheld-XRF instruments, and with EPMA, PIXE, SIMS. Hence, nanopellets proved to be a new and, possibly, universal matrix-matched MRM for many custom solid materials to be used with many in situ analytical techniques.
In addition, this way of sample preparation bears the potential of completely replacing conventional tedious and time-consuming wet-chemistry procedures for bulk analysis, and this holds true in particular for refractory samples like ceramics, granites, ultramafic rocks, and samples with volatile or easy-to-contaminate components (e.g., B). Here we give an overview of the present state of development of new MRM[3] and their characterization in terms of grain size distribution, surface topography, porosity, homogeneity, and accuracy of analytical results for both elemental (major, minor, trace and ultra-trace elements) and isotopic (Sr, Li, B, O) composition.

[1 ] Garbe-Schönberg D & Müller S, JAAS, 29, 990 (2014); [2] Hogmalm KJ, et al., JAAS, 32, 305 (2017); [3] www.my-standards.com; see also paper by D. Savard et al., this conference
Keywords: reference materials
  • Lecture (Conference)
    Geoanalysis 2018, 08.-13.07.2018, Sydney, Australia

Permalink: https://www.hzdr.de/publications/Publ-27281
Publ.-Id: 27281


Theoretical Modelling of High-Resolution X-Ray Absorption Spectra at Uranium M4 Edge

Kolorenc, J.; Kvashnina, K.
We investigate the origin of satellite features that appear in the high-resolution x-ray absorption spectra measured at the uranium M4 edge in compounds where the uranium atoms are in the U6+ oxidation state. We employ a material-specific Anderson impurity model derived from the electronic structure obtained by the density-functional theory.

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Publ.-Id: 27280


Experimental investigation of three-dimensional bubbly two-phase pipe flows

Neumann, M.; Bieberle, A.; Krepper, E.; Hampel, U.
Modelling gas-liquid two-phase flow is a topic of constant relevance in nuclear thermal hydraulics. Gas-disperse two-phase flows occur in e.g. fuel elements in the reactor core, in pipes and components during pressure loss, sudden reflooding or other events. Due to the deformable gas-liquid interface and the complexity of heat, mass and momentum transfer across the interface, gas-liquid two-phase flow is very difficult to model and simulate. On the device scale it is common to use Euler/Euler multi-fluid approaches for CFD simulations, which require a good number of empirical correlations as closure models. Such models are commonly derived from experiments. Validation of the correctness of predictive simulations then also requires experiments, which must be simplified to a degree to allow provision of CFD-grade experimental data but complex enough to resemble real flow situations. The latter calls especially for investigations on flow fields in more complex three-dimensional domains, which are prototypical for e.g. bends, valves, T-junctions and rod bundles.
In this contribution the experimental investigation of generic three-dimensional two-phase flows will be presented. Experiments were performed at a vertical test section at the Transient Two-Phase Flow (TOPFLOW) facility at Helmholtz-Zentrum Dresden – Rossendorf (HZDR). The test section is a pipe with an inner diameter of 54 mm and a length of 5000 mm with a flow constriction at half lengths. For the latter a ring shaped diaphragm and a half-moon shaped diaphragm have been investigated. Experiments were performed for a wide range of superficial gas and liquid velocities in the bubbly flow regime. Besides conventional measurement techniques for mass flow rates, temperatures and pressure, the ultrafast X-ray tomography scanner ROFEX for the determination of bubble dynamics, as well as a specifically adapted thermal anemometer probe for determination of liquid velocities is employed. The two-phase flow in such geometry exhibits certain important structures. In the narrow obstacle passage the flow accelerates with accordingly high shear stress being visible in large bubble deformation and break-up. Downstream a dead zone with recirculation develops and bubbles are being captured, which is associated with increased gas hold-up and bubble coalescence. The high resolution measurements allow for the first time to study the two-phase dynamics in detail and disclose velocity distributions along with gas phase and bubble size data as a function of time and space.
Keywords: two-phase flow, three-dimensional flow field, ultrafast X-ray tomography, thermal anemometry
  • Contribution to proceedings
    17th International Topical Meeting on Nuclear Reactor Thermal Hydraulics (NURETH-17), 03.-08.09.2017, Xi'an, China
  • Lecture (Conference)
    17th International Topical Meeting on Nuclear Reactor Thermal Hydraulics (NURETH-17), 03.-08.09.2017, Xi'an, China

Permalink: https://www.hzdr.de/publications/Publ-27279
Publ.-Id: 27279


Two-Phase Flow Studies in Complex Geometries

Neumann, M.; Hampel, U.
This contribution describes an experimental study on generic three-dimensional two-phase flows. The experiments are conducted at the Transient Two-Phase Flow (TOPFLOW) facility at Helmholtz-Zentrum Dresden – Rossendorf (HZDR) and are a continuation of earlier studies, which were performed using a moveable flow obstacle and the wire-mesh sensor technique [1]–[3]. Although these investigations already provided very new data from a complex two-phase flow, the required minimal intrusiveness of both sensor and obstacle motion unit lead to some non-idealities with respect to the fully undisturbed flow. With a new imaging technique, ultrafast electron beam X-ray tomography, we are now able to perform investigations fully non-intrusively and to study the gas phase dynamics with high temporal and spatial resolution in two planes simultaneously. First results of the experimental study are presented here.
  • Contribution to proceedings
    48th Annual Meeting on Nuclear Technology, 16.-17.05.2017, Berlin, Deutschland
    Proceedings of the 48th Annual Meeting on Nuclear Technology

Permalink: https://www.hzdr.de/publications/Publ-27278
Publ.-Id: 27278


Experimental investigation of three-dimensional disperse two-phase flow

Neumann, M.; Bieberle, A.; Hampel, U.
In vielen industriellen Prozessen und Apparaten treten Mehrphasenströmungen auf. Dies sind häufig Flüssigkeits-Gas-Strömungen, beispielsweise in der Kraftwerkstechnik, in Wärmetauschern, chemischen Reaktoren und Trennapparaten oder in Ölfördersystemen. Die Berechnung solcher Strömungen mittels computergestützter Simulationswerkzeuge (CFD-Codes), etwa zur Unterstützung der Auslegung, Optimierung und Sicherheitsbewertung, ist ein großes Ziel, welches aber schwierig zu erreichen ist, da die Physik von Zweiphasenströmungen im Vergleich zu einphasigen Strömungen um ein Vielfaches komplexer ist. Grund dafür ist die Komplexität der Transportprozesse über stark verformbare und sich verändernde Phasengrenzflächen in mehreren Zeit- und Längenskalen. Zudem werden durch anlagentechnische Komponenten, wie beispielsweise Krümmer, Ventile, T-Stücke oder querschnittsverändernde Einbauten, ausgeprägte dreidimensionale Strömungsfelder erzeugt, welche von aktuellen CFD-Codes nur sehr stark eingeschränkt berechnet werden können.
Der Beitrag beschäftigt sich mit der experimentellen Untersuchung von generischen dreidimensionalen Zweiphasenströmungen. Mit Hilfe neuartiger experimenteller Methoden soll dabei eine Datenbasis für die nachhaltige Validierung und Weiterentwicklung von CFD-Codes, speziell für dreidimensionale Strömungseffekte, erzeugt werden.
  • Poster
    Jahrestreffen der ProcessNet-Fachgruppen Mehrphasenströmungen, Partikelmesstechnik, Zerkleinern und Klassieren, Computational Fluid Dynamics, Mischvorgänge und dem TAK Aerosoltechnologie, 14.-17.03.2017, Dresden, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-27277
Publ.-Id: 27277


Developing a Single Plane Compton Camera for Radionuclide Imaging

Deneva, B.; Roemer, K.; Wagner, A.; Enghardt, W.; Pausch, G.; Koegler, T.
Anger cameras are still the primary technology for radionuclide imaging in nuclear medicine [1]. Despite the achieved advances in improving the image quality over the past 60 years since its invention [2], there are physical limits to the camera performance (limited detection efficiency, decreasing spatial resolution of high energetic gamma rays, fixed dependency of the spatial resolution and detection efficiency from the used collimator). In order to overcome these limitations, the concept of the “Single Plane Compton Camera” (SPCC, see also Ref. [3]) was developed. The SPCC is based on the idea of the “Directional Gamma Radiation Detector” published in Ref. [4] and [5].
A setup for the investigation of the SPCC concept was developed recently at the Helmholtz-Zentrum Dresden - Rossendorf. Based on a GAGG:Ce (Gadolinium Aluminum Gallium Garnet, Gd3Al2Ga3O12) scintillator array and read out by digital silicon photomultipliers the setup is intend to deliver spatial information of activity distributions. The authors will present first experimental results acquired with the new setup and will compare them to predictions obtained from particle transport calculations performed with GEANT 4 [6].
[1] S. R. Cherry, J. A. Sorenson and M. E. Phelps, Physics in Nuclear Medicine, 4th ed., Elsevier, 2013.
[2] H. Anger, "A new instrument for mapping gamma ray emitters," Biology and Medicine Quaterly Report, 1957.
[3] G. Pausch et al., Paper N60-1 presented at the 2016 IEEE NSS/MIC in Strasbourg, France, Conference Record
[4] G. Kraft et al., U.S. patent no. 8030617 B2, granted in Oct. 2011
[5] A. Gueorguiev et al. U.S. patent no. 8299441 B2, granted in Oct. 2012
[6] A. Allison, "Geant 4 - a simulation toolkit", Nucl. Instr. and Meth. A. 506, (2003) 250-303
Keywords: Radionuclide imaging, Single Plane Compton Imaging, SPCI, radiation detector
  • Open Access Logo Contribution to proceedings
    49. Jahrestagung der Deutschen Gesellschaft für Medizinische Physik, 19.-22.09.2018, Nürnberg, Deutschland

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Permalink: https://www.hzdr.de/publications/Publ-27276
Publ.-Id: 27276


Preyssler-Pope-Jeannin Polyanions [NaP5W30O110]14- and [AgP5W30O110]14-: Synthesis, Structural Characterization, Electrochemistry, Antiproliferative and Antibacterial Activity

Haider, A.; Zarschler, K.; Joshi, S. A.; Smith, R.; Lin, Z.; Mougharbel, A.; Herzog, U.; Müller, C. E.; Stephan, H.; Kortz, U.
The Preyssler-Pope-Jeannin polyanion [NaP5W30O110]14- (1) has been prepared by microwave-assisted synthesis in only 2 h with a yield comparable to the reported hydrothermal procedure. The purity of 1 was confirmed by FT-IR and multinuclear NMR (31P, 183W) analysis. The silver(I)-containing analogue [AgP5W30O110]14- (2) has also been prepared by hydrothermal (6 d) as well as microwave-based (2 h) procedures. Polyanion 2 was characterized in the solid state by FT-IR, single-crystal XRD, TGA, and elemental analysis and in solution by 31P and 183W NMR, electrochemistry and ESI-MS. The antiproliferative activities against human cells as well as the antimicrobial properties towards Gram-positive and Gram-negative bacteria were comparatively evaluated for 1 and 2.
Keywords: Polyoxoxmetalates; Microwave-Assisted Synthesis; Nuclear Magenetic Resonance (NMR); Bioactivity

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Permalink: https://www.hzdr.de/publications/Publ-27275
Publ.-Id: 27275


Performance demonstration of the PEnELOPE main amplifier HEPA I using broadband nanosecond pulses

Albach, D.; Loeser, M.; Siebold, M.; Schramm, U.
We report on the energetic and beam quality performance of the second to the last main amplifier section HEPA I of the PEnELOPE laser project. A polarization coupled double-12-pass scheme to verify the full amplification capacity of the last two amplifiers HEPA~I and II was used. The small signal gain for a narrow band cw laser was 900 and 527 for a broadband nanosecond pulse, demonstrating 12.6 J of output pulse energy. Those pulses, being spectrally wide enough to support equivalent 150 fs long ultrashort pulses, are shown with an excellent spatial beam quality. A first active correction of the wavefront using a deformable mirror resulted in a Strehl ratio of 76 % in the single-12-pass configuration for HEPA I.
Keywords: Diode-pumped lasers; ytterbium; laser amplifiers; laser diagnostics; pulse energy

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Publ.-Id: 27274


Reactive transport modeling using heterogeneous flow field data based on positron emission tomography

Lippold, H.; Kulenkampff, J.; Karimzadeh, L.; Stuhlfauth, C.; Lippmann-Pipke, J.; Fischer, C.
Discrepancies between experimental and RTM results are often attributed to flow field heterogeneities. Positron emission tomography (PET) provides direct and quantitative insight into flow fields in complex media, such as barrier materials or porous rocks.
Adsorption and transport of the herbicide 2-methyl-4-chlorophenoxyacetic acid (MCPA) in a homogeneous sand-goethite system were investigated as a function of pH. Interaction of MCPA with the solid surface was geochemically modeled using the charge distribution multisite complexation (CD-MUSIC) approach. Based on this calibrated surface complexation model, retardation of MCPA in transport experiments was significantly underestimated by 1D simulations with hydrodynamic parameter values obtained from a fit to the breakthrough of HTO as a conservative tracer.
On the basis of flow field data derived from PET measurements, heterogeneous flow observed for 18F as a tracer was reproduced in 2D simulations (with flow velocities controlled by the pressure gradient field according to Darcy’s law) assuming a peripheral zone with increased porosity and permeability. Using this flow model, the predicted breakthrough of MCPA was significantly more realistic compared to 1D simulations with the same chemical parameter values. Thus, this study demonstrates quantitatively that inconsistencies between static (batch) and dynamic (column) systems can be caused by heterogeneities in fluid flow, i.e., not necessarily by non-equilibrium conditions. This in turn highlights the need to consider real flow fields in predictive transport models.
  • Lecture (Conference)
    Goldschmidt 2018, 12.-17.08.2018, Boston, United States of America

Permalink: https://www.hzdr.de/publications/Publ-27273
Publ.-Id: 27273


Magnetic field-induced proton dose enhancement: Experimental verification and Monte-Carlo simulation

Lühr, A.ORC; Burigo, L. N.; Gantz, S.; Schellhammer, S.; Hoffmann, A. L.
Introduction
Proton therapy (PT) is expected to benefit from integration with magnetic resonance (MR) imaging. However, the magnetic field distorts the dose distribution and induces a local dose enhancement at tissue-air interfaces by the electron return effect (ERE). For MR-integrated photon therapy, a dose enhancement ratio (DER) of 40% compared to no magnetic field has been reported. Here, measurements and calculations of DER for proton beams in transverse magnetic fields are reported.

Methods
Two measurement setups were used: EBT3 films were either attached to the distal face of one or sandwiched between two 10 mm PMMA slabs. Films were irradiated with a 200 MeV proton beam, both with and without transverse magnetic field (0.92 T). High-resolution Monte-Carlo simulations were used to reproduce the experimental findings and to calculate the DER for proton energies between 50−200 MeV and magnetic field strengths between 0.35−3 T within the first 0.05 mm (DERmax) and as function of distance from the air interface.

Results
A DER of (2.2±0.4)% and (0.5±0.6)% was measured at 0.156 and 0.467 mm from the interface, respectively (Fig.1). Measurements and simulations agreed within 0.15%. Simulations using a 200 MeV beam showed a DERmax of 2.6% and 8.2% for 0.35 and 1.5 T, respectively (Fig.2). At 1 T, DERmax increased from 3.2% to 7.6% between 50 and 200 MeV.
Conclusion
For proton beams, the ERE in transverse magnetic fields is measurable. The dose enhancement is well predictable, decreases with distance from the interface, and is negligible after 1 mm. Although small, the impact of the ERE cannot be ignored for dosimetry with air-filled ionization chambers and in porous media (e.g. lung treatment).
Keywords: proton therapy, magnetic resonance imaging, MRI, MR, radiotherapy, dosimetry, electron return effect
  • Abstract in refereed journal
    TBD (2018)

Permalink: https://www.hzdr.de/publications/Publ-27272
Publ.-Id: 27272


Synthesis and radiofluorination of novel fluoren-9-one based derivatives for the imaging of α7 nicotinic acetylcholine receptor with PET

Teodoro, R.; Scheunemann, M.; Wenzel, B.; Peters, D.; Deuther-Conrad, W.; Brust, P.
By structure-activity relationship studies on the tilorone scaffold, the ‘one armed’ substituted dibenzothiophenes and the fluoren-9-ones were identified as the most potential α7 nAChR ligands. While the suitability of dibenzothiophene derivatives as PET tracers is recognized, the potential of fluoren-9-ones is insufficiently investigated. We herein report on a series of fluoren-9-one based derivatives targeting α7 nAChR with compounds 8a and 8c possessing the highest affinity and selectivity. Accordingly, with [18F]8a and [18F]8c we designed and initially evaluated the first fluoren-9-one derived α7 nAChR selective PET ligands. A future application of these radioligands is facilitated by the herein presented successful implementation of fully automated radiosynthesis.
Keywords: α7 nAChR PET Radiofluorination Fluoren-9-one Dibenzothiophenes

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Permalink: https://www.hzdr.de/publications/Publ-27271
Publ.-Id: 27271


Consolidation of surface speciations by a combined spectroscopic and modeling approach

Foerstendorf, H.ORC; Jordan, N.; Heim, K.; Mayordomo, N.; Steudtner, R.; Stockmann, M.
A reliable risk assessment of a deep geological waste disposal site for spent nuclear fuel refers to thermodynamic data bases which must contain resilient data sets. This information can be obtained from Surface Complexation Modeling (SCM) of batch sorption data, which is in turn consolidated by molecular information of relevant, prevailing species at mineral surfaces derived from spectroscopic investigations.
A combined approach of optical spectroscopic techniques, such as vibrational and luminescence spectroscopy, classical batch sorption studies and SCM was applied for the study of the surface speciation of actinide- and selenium oxyanions on mineral phases. In this study, spectroscopic findings of the surface speciation of uranium(VI) and selenium(IV) and (VI) on different mineral oxide phases, serving as models for complex naturally occurring minerals in a host rock of a nuclear waste repository, are presented.
From the ternary sorption system U(VI)/phosphate/SiO2, the formation of two binary uranyl surface species and of a precipitate was found to be sufficient to satisfactorily fit the respective batch results by SCM. For the selenium(IV) and selenium(VI) binary sorption systems, a single predominant inner-sphere selenite and outer-sphere selenate surface species on alumina phases were identified by vibrational spectroscopy, respectively. With respect to the bidentate binding mode observed for both oxyanionic surface species, SCM provided excellent fitting results of the batch sorption data.
The results of this study demonstrated that the combined approach of in situ spectroscopy and batch sorption studies contributes to an improved performance of future assessments for the migration of radionuclides an fission products in the environment of a repository site.
  • Lecture (Conference)
    Goldschmidt 2018, 12.-17.08.2018, Boston, U.S.A.

Permalink: https://www.hzdr.de/publications/Publ-27270
Publ.-Id: 27270


Einfluss der Bildgebung eines in beam MR-Scanners auf die Dosisprofile eines Protonenstrahls

Karsch, L.; Gantz, S.; Pawelke, J.; Schellhammer, S.; Smeets, J.; Hoffmann, A.
Einleitung
Eine in Echtzeit ausgeführte Magnetresonanztomografie (MRT) könnte die geometrische Präzision der Protonentherapie künftig verbessern. Zur MR-Bildgebung werden jedoch magnetische Gradientenfelder in Pulssequenzen auf- und abgebaut, die mit den Protonen wechselwirken. Aufgrund der geringen Stärke der Gradientenfelder wird theoretisch keine Änderung der Dosisverteilung des Protonenstrahls durch diese magnetischen Felder erwartet. Ziel dieser Arbeit war einerseits die Entwicklung eines Aufbaus zur gleichzeitigen Strahldetektion und MR-Bildaufnahme und andererseits die experimentelle Untersuchung der Beeinflussung des Protonenstrahls durch die gleichzeitige MR-Bildgebung.

Material & Methoden
Ein offener 0.22 T MR-Scanner (MrJ2200, Paramed) wurde an einer horizontalen Protonenstrahlführung installiert, so dass der Protonenstrahl auf das magnetische Isozentrum des MR-Scanners gerichtet ist. Um den Einfluss der MR-Bildgebung auf den Protonenstrahl zu untersuchen wurden zwei Experimente mit unterschiedlichen Aufbauten und MR-Pulssequenzen durchgeführt.
Im Absorptionsexperiment wurde im Isozentrum des MR-Scanners ein mit Flüssigszintillator (BC517H, Saint Gobain) gefülltes Phantom aus PMMA platziert. Das vom bestrahlten Szintillator emittierte Licht wurde mittels einer Kamera aufgezeichnet. Aus den Kamerabildern wurde auf die statistische Genauigkeit des Verfahrens geschlossen und diese mit der Differenz der über mehrere Aufnahmen gemittelten Dosisprofile verglichen.
Beim Transmissionsexperiment wurde auf ein bildgebendes Phantom verzichtet und die Dosisprofile ca. 1 m hinter dem Isozentrum des MR-Scanners mit einem Festkörper-Szintillator basierten 2D-Detektor (Lynx, IBA) aufgezeichnet. Die gemessenen Dosisprofile wurden durch eine gedrehte zweidimensionale Normalverteilung angenähert.

Ergebnisse
Im Absorptionsexperiment liegen die Unterschiede in den Pixelwerten der Kamerabilder zwischen laufender und ausgeschalteter MR-Bildgebung innerhalb der statistischen Schwankungen. Auch im Transmissionsexperiment zeigen die fünf Anpassungsparameter der Normalverteilung keine Änderung in den Dosisprofilen durch die Bildaufnahme des MR-Scanners.

Zusammenfassung
Gleichzeitige Detektion des Protonenstrahles während einer MR-Bildaufnahme ist mit Hilfe von Phantomen, die mit Flüssigszintillator gefüllt sind, möglich. Die einzelnen MR-Pulssequenzen zeigen keinen Einfluss auf den Protonenstrahl, so dass in der Bestrahlungsplanung einer MR-integrierten Protonentherapie nur das statische Magnetfeld des MR-Scanners berücksichtigt werden muss.
Keywords: MR, Radiation Therapy, Proton Therapy
  • Poster
    49. Jahrestagung der Deutschen Gesellschaft für Medizinische Physik, 19.09.2018, Nürnberg, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-27269
Publ.-Id: 27269


Quantitative Measurement of Interaction between Solidification and Convection in Ammonium-Chloride Solutions

Anders, S.; Noto, D.; Eckert, S.
An experimental investigation of double-diffusive convection with simultaneous crystallisation in ammonium-chloride solutions will be presented. Measurements were performed in a transparent Hele-Shaw with controlled thermal boundary conditions. The flow field of the liquid was measured by PIV. Using thermochromic liquid crystals, the temperature field inside the fluid was established. PTV was used to determine the size-evolution and the trajectories of the salt crystals. Alternating lighting methods and digital image filtering allow for simultaneous operation of PIV, PTV and temperature field measurement. This enables a quantitative study of the interplay of convection regimes and solidification processes like columnar and equiaxed crystallization, chimney-formation and remelting.
Keywords: Iron Snow, PTV, PIV, TLC, Multiphase Flow, Solidification, Double-diffusive Convection
  • Lecture (Conference)
    Symposium zur Simulation Metallurgischer Prozesse 2018, 30.01.-02.02.2018, Feuerkogel, Österreich

Permalink: https://www.hzdr.de/publications/Publ-27268
Publ.-Id: 27268


The mineralogy of weathering products of Bi-bearing tennantite – clues for the process and the mobilisation of heavy metals and toxic elements

Keim, M.; Staude, S.; Marquardt, K.; Bachmann, K.; Opitz, J.; Markl, G.
Since the complex sulfosalts of the tennantite-tetrahedrite solid-solution series [(Cu,Ag)6Cu4(Fe,Zn,Cu,Hg,Cd)2(Sb,As,Bi,Te)4(S,Se)13] are widespread in many geological environments and accommodate heavy metals and toxic elements, a better understanding of the general weathering process and mobility of elements are important to evaluate environmental risks. In this study, the weathering of Bi-rich members of this mineral group were investigated in detail using microscopy, EMPA, SEM, TEM, LA-ICP-MS, Raman, µXRD and MLA. Observation reveal a subdivision in four temporally distinguishable weathering stages, spatially attributed to weathering environments of different chemical potentials. During the first stage, weathering occurs as tubes within the fahlore producing a phase assemblage of nm-sized roméite group minerals, tripuhyite, a crystalline Cu-oxide phase and crystalline Cu-sulfides. The textural appearance and the occurrence of these secondary sulfide indicates a low oxidation potential during this stage, typical for cementation zones. Mass balance calculations show that during this stage As, Zn and partially S are released to the weathering fluids. In contrast, Sb, Bi, Fe, S and Cu are stored in the roméite group minerals, tripuhyite, the copper oxide phase, and sulfides. During weathering stage 2, amorphous and nano-crystalline arsenates were formed replacing fahlore in most cases as weathering fronts. Their textures indicate a fluid with higher oxidation potential than in stage 1, typical for oxidation zones. The occurrence of arsenates shows that arsenic in contrast to stage 1 behaves immobile during this stage. Bismuth behaves immobile and is stored in the amorphous nano-crystalline phase. Mass balance calculations reveal that Zn, Sb, and S and partially Cu are lost, whereas Fe is added. Weathering stage 3 occurs only locally and reflects processes in micro compartments that are different for each locality and not characteristic for the general weathering process including the dissolution of former phases but also precipitation of new ones such as amorphous Cu-silicates. Stage 4 is characterized by the formation of crystalline Cu-Ba-Ca-Al-arsenates and Cu-carbonates mostly along cracks and in voids, spatially independent of the precursor fahlore. This stage reflects the increasing importance of the local geology, host rock and gangue mineralogy on weathering, typical in near surface environments of oxidation zones, where elements are highly mobile and a high fluid rock ratio is realized.
Keywords: Tennantite-tetrahedrite, weathering, bismuth, cementation zone, oxidation zone, Schwarzwald

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Publ.-Id: 27267


Applied Mineralogy for Resource Efficiency of Platinum Metals - Towards a Geometallurgical Model

Bachmann, K.; Menzel, P.; Tolosana-Delgado, R.; Gutzmer, J.
A geometallurgical model allows to predict parameters relevant for mineral beneficiation in a spatial domain. Therefore, we need a basic understanding of the geolocial architecture which can be provided by 3D geological models. Additionally, a tailored sample selection and characterization is crucial. This may include drill core logging data, whole rock geochemistry, modal mineralogies, micro-textures and mineral association as well as mineral chemistry data. In a next step, it is necessary to integrate the data into a spatial context and to derive process-relevant paramters. Finally, the development of domains with similar mineral beneficiation characteristics as well as geostatistical interpolation of relevant parameters onto a 3D geometry is possible.
  • Invited lecture (Conferences)
    Joint AMREP & DST-CIMERA Symposium, 14.-15.03.2018, Johannesburg, South Africa

Permalink: https://www.hzdr.de/publications/Publ-27266
Publ.-Id: 27266


Microbial diversity and activity in rock salt formations

Cherkouk, A.; Bader, M.; Bachran, M.; Swanson, J. S.; Steudtner, R.; Drobot, B.; Schmidt, M.; Musat, N.; Rossberg, A.; Ikeda-Ohno, A.; Stumpf, T.
Rock salt formations are considered as potential host rocks for the long-term storage of highly radioactive waste in a deep geological repository. A combination of culture-dependent and culture-independent methods was used to investigate the microbial diversity in rock salt. Extremely halophilic archaea, e.g. Halobacterium species, dominate this habitat. For long-term risk assessment it is of high interest to study how these microorganisms can interact with radionuclides if released from the waste repository. Therefore, the interactions of the extremely halophilic archaeon Halobacterium noricense DSM 15987T with uranium, one of the major radionuclides of concern in the geological repository, were investigated in detail in batch experiments. A multi-spectroscopic and microscopic approach was used to decipher the interaction mechanisms on a molecular level. H. noricense DSM 15987T showed a multistage bioassociation of uranium. By using time-resolved laser-induced fluorescence spectroscopy and X-ray absorption spectroscopy the formation of U(VI) phosphate minerals, such as meta-autunite, was observed. Furthermore, the presence of U(VI)-phosphate mineral could be visualized by scanning electron microscopy. These findings highlight the potential significance of the microbial life in deep geological hypersaline environments and offer new insights into the microbe-actinide interactions at highly saline conditions relevant to the disposal of highly radioactive waste as well as bioremediation.
  • Poster
    ISME17 - 17th International Symposium on Microbial Ecology, 12.-17.08.2018, Leipzig, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-27265
Publ.-Id: 27265


Variation in PGM and BMS assemblages in the LG-6 and LG-6A chromitites of the western Bushveld Complex, South Africa

Bachmann, K.; Osbahr, I.; Tolosana-Delgado, R.; Chetty, D.; Gutzmer, J.
This study focuses on the LG-6 and LG-6A chromitite seams at the Thaba mine located on the western limb of the Bushveld Complex. Platinum group minerals and base-metal sulfides are studied by mineral liberation analysis and electron microprobe analysis to define distinct assemblages and to evaluate the potential for beneficiation. Two distinct major mineral assemblages are defined: The first assemblage is rich in PGE-sulfides and alloys of Fe and Sn as well as chalcopyrite, pentlandite while second assemblage is rich in PGE-sulfarsenides and -arsenides and -alloys of Sb and Bi, pentlandite and Co-rich pentlandite.
  • Contribution to proceedings
    International Platinum Symposium, 30.06.-06.07.2018, Polokwane, South Africa

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Permalink: https://www.hzdr.de/publications/Publ-27264
Publ.-Id: 27264


PGE Distribution and Mineralogy in the LG-6 and Middle Group Chromitite Layers, Thaba Mine, Bushveld Complex

Kaufmann, F.; Hecht, L.; Bachmann, K.; Trumbull, R.; Veksler, I.; CRONIMET Chrome Mining (Pty.) Ltd.
Here we present information about concentrations, distribution and mineralogy of platinum group elements (PGE) in the sequence of chromitite layers from LG-6 to MG-4 at the Thaba mine in the north-western sector of the Bushveld Complex in South Africa. The information is based on assay analyses of drill core samples and studies of platinum group minerals and base-metal sulfides by mineral liberation analysis. Total concentrations of PGE gradually increase with the stratigraphic height from the LG-6 layer to MG-4. Detailed sampling of the LG-6, LG-6A, MG-1 and MG-2 layers revealed uneven vertical distribution of PGE with the highest concentrations at the footwall contacts. Pt-Pd ratios vary broadly from one layer to another and tend to increase from top to bottom within the individual layers. The assemblage of platinum group minerals in the LG-6 and LG-6A layers comprises equal proportions of (Pt,Pd)S, malanite and laurite, and minor amounts of Fe-Sn alloys sperrylite. PGE tellurides and bismuthotellurides are largely absent. In contrast, the PGE mineralogy of the MG-1 and MG-2 layers is dominated by laurite.
  • Contribution to proceedings
    International Platinum Symposium, 30.06.-06.07.2018, Polokwane, South Africa

Permalink: https://www.hzdr.de/publications/Publ-27263
Publ.-Id: 27263


Spatially-resolved characterization of Eu(III) interaction with granitic rock (Eibenstock, Germany)

Schmidt, M.ORC; Molodtsov, K.
The mobility of (radio-)contaminants in the geosphere is controlled by their interaction with the surfaces of surrounding minerals. Typically these interactions are studied either with single mineral phases, or in field studies in natural rock formations consisting of multiple mineral phases. In the former case, the involved reactions can be characterized at the molecular level with appropriate spectroscopic tools, but the complexity of the natural rock is lost, while the latter case often only allows a quantitative approach due to the inherent complexity of the natural system.
Here we present a novel approach to bridge this gap in the understanding of sorption processes. Time-resolved laser-induced fluroescence spectroscopy (TRLFS) is a well established technique to characterize the speciation of luminescent metal ions, e.g Eu(III)[1] or Cm(III).[2] We have adapted the technique to allow scanning a rock sample consisting of a variety of mineral grains, through a focused laser beam with a spatial resolution ~ 20 µm (µTRLFS). This way we are able to obtain full emission spectra and lifetimes in each spot. Through this improvement, it is possible to not only map the distribution of a fluorescent probe on the rock, but also to determine its speciation in each location, with respect to its coordination strength and hydration state.
The interaction of Eu(III) with granitic rock thick sections from the former uranium mine Eibenstock, Germany, were investigated by µTRLFS. The investigation is complemented by mineral characterization using µXRF, EMPA, and thin section microscopy. The results clearly show the differing sorption capacity and sorption strength of the minerals contained in the granite, with the highest sorption capacity found for feldspars. In addition, grain boundaries often show a reactivity distinct from both bordering mineral grains, e.g. a quartz/biotite grain boundary showing higher adsorption than both, quartz and biotite.
In summary, the results highlight the necessity to complement studies of model systems with more realistic whole system investigations. The technical improvement to a well-established spectroscopic tool also offers opportunities for other fields of (bio)geochemistry.

(1) Binnemans, K., Coord. Chem. Rev. 2015, 295, 1-45.
(2) Edelstein, N.M., Coord. Chem. Rev. 2006, 250, 948-973.
Keywords: TRLFS, europium, sorption, granite, microscopy, µTRLFS
  • Lecture (Conference)
    Goldschmidt 2018, 12.-17.08.2018, Boston, USA

Permalink: https://www.hzdr.de/publications/Publ-27262
Publ.-Id: 27262


Regge Trajectories of Radial Meson Excitations: Exploring the Dyson-Schwinger-- Bethe-Salpeter Approach

Greifenhagen, R.; Kämpfer, B.; Kaptari, L. P.
The combined Dyson-Schwinger and Bethe-Salpeter equations in rainbow-ladder approximation are used to search for Regge trajectories of mesons in the pseudo-scalar and vector channels. We focus on the often employed Alkofer-Watson-Weigel kernel which is known to deliver good results for the ground state meson spectra; it provides linear Regge trajectories in the JP=0− channel.

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Permalink: https://www.hzdr.de/publications/Publ-27261
Publ.-Id: 27261


Impact of Dipolar Interaction on Superfluid Spin Transport

Schneider, T.; Barsukov, I.; Smith, A.; Upadhyaya, P.; Liu, Y.; Fan, Y.; Wang, K.; Macdonald, A.; Tserkovnyak, Y.; Krivorotov, I. N.
Ferromagnetic easy-plane system are theoretically excepted to support a long-range coherent transport flow, normally referred as spin superfluid. However, the influence of local dipole-dipole interaction on these states are not fully investigated. Here, the present a detailed micromagnetic study of the superfluid flow in a easy-plane ferromagnetic in the presence of local dipole-dipole interactions.
  • Lecture (others)
    Spintronics group seminar, 15.03.2018, Irvine, CA, USA
  • Lecture (others)
    Group seminar Prof. Tserkovnyak, 19.03.2018, Los Angeles, USA

Permalink: https://www.hzdr.de/publications/Publ-27260
Publ.-Id: 27260


Charakterisierung der MR-Relaxations- und Bewegungseigenschaften eines 4D MRT Phantoms im Rahmen der Kommissionierung an einem 3T MR Scanner

Schneider, S.; Dolde, K.; Engler, J.; Hoffmann, A. L.; Pfaffenberger, A.
Einleitung
Für die klinische Etablierung von Magnetresonanztomographen (MRT) in der bildgestützten Strahlentherapie, allen voran der hybriden MR-Linacs, bedarf es der Analyse und regelmäßiger Qualitätssicherung der Bewegungscharakterisierung auf Basis der MRT Bilder. Ziel dieser Studie war die Kommissionierung eines programmierbaren 4D MRT-Bewegungsphantoms bezüglich seiner bildgebenden MR-Relaxations- und Bewegungseigenschaften an einem 3T MRT und die Entwicklung einer Methode zur automatisierten Qualitätssicherung von MRT-Sequenzen zur Bewegungsanalyse.
Material & Methoden
Das MRI-LINAC Dynamic Phantom (Model 008M, CIRS) wurde mit Mineralöl (Marcol Blend, Philips) gefüllt und mit einer Hilfskonstruktion auf einer flachen Tischauflage (Medibord Ltd) positioniert. Messungen wurden an einem 3.0T MRT (Ingenuity TF PET/MR, Philips) durchgeführt. Mittels MR-Relaxometrie wurden die Relaxationszeiten des Gel-gefüllten beweglichen Zylinders und des Targets bestimmt. Die T1-Relaxationszeit wurde durch eine Inversion-Recovery Spin-Echo (IR-SE) Methode , die T2-Relaxationszeit durch eine Multi-Echo Gradient-and-Spin-Echo (GraSE) berechnet. Sinusförmige 1D, 2D und 3D Target-Trajektorien mit patiententypischen Organauslenkungen (5-40mm) und Frequenzen (0.1-0.2Hz) sowie eine 1D Patientennavigator Atemkurve wurden im Phantom generiert und mittels 2D-cine MR Sequenzen (Zeitauflösung von <0.5s) aufgenommen. Mit einer selbst entwickelten MATLAB-basierten Tracking-Software wurden die 2D-cine Bilder automatisiert analysiert.
Ergebnisse
Die Relaxationsparameter für Zylinder (T1=871±36ms / T2=13.4±1.3ms) und Target (T1=208±2.8ms / T2=30.5±0.7ms) wurden bestimmt. Die extrahierten Amplituden der Sinustrajektorien zeigen Abweichungen zu den eingestellten Werten von <0.4mm in AP/LR und <0.2mm in IS Richtung, während die Frequenzen mit Abweichungen von <0.001Hz bestimmt wurden. Die Navigatorkurve konnte mit einer mittleren Amplitudenabweichung von 0.3mm bestimmt werden, bei einer maximalen Abweichung von <1.0mm.
Zusammenfassung
Das 4D-Phantom wurde an einem klinischen 3T MRT bezüglich seiner Relaxationseigenschaften und der Möglichkeit einer 3D Bewegungsanalyse kommissioniert. Der entwickelte Aufbau und die Methodik erlauben regelmäßige Qualitätskontrollen der Bewegungscharakterisierung auf MR-Basis.
Keywords: MRT, Bewegungs-Phantom, Kommissionierung
  • Poster
    49. Jahrestagung der Deutschen Gesellschaft für Medizinische Physik und 21. Jahrestagung der Deutschen Sektion der ISMRM, 19.-22.09.2018, Nürnberg, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-27259
Publ.-Id: 27259


Interaction of fluid flow with heat and mass transfer in Liquid Metal Batteries

Personnettaz, P.; Landgraf, S.; Nimtz, M.; Weber, N.; Weier, T.
Liquid metal batteries (LMBs) are suggested as a possible solution of the energy storage problem. An LMB consists of three stably stratified layers, two liquid metals are separated by a molten salt electrolyte.
Operation was so far demonstrated for small prototypes only. In order to upscale cells to a viable commercial scale a deep knowledge of the physics involved is required.
The relatively simple chemistry and geometry, the presence of multiple and multi-physics phenomena and the completely fluid nature of the active materials have made the LMB an intriguing candidate for continuum mechanics studies.
The cell is in fact subject to a coexistent transport of mass, heat, charge and momentum together with chemical and electrochemical reactions.
The fluid flow that naturally occur can be beneficial if it is able to improve the mass transport, delaying the formation of solid intermetallic phases.
In our work the attention is focused on heat and mass transfer. The continuum balances are defined in general terms, taking into account the electrochemical nature of the system. The corresponding scalar fields (e.g. temperature and solute concentration) are then computed with pure diffusive models. In a second step the interaction with the induced fluid flow is taken into account. Thermal convection in Li||Bi LMBs is studied with an improved version of the multiphase VOF solver multiphaseInterFOAM. Advection-diffusion mass transfer is investigated in the positive electrode with single-phase CFD solvers.
The first results of thermo-solutal convection are presented, the modeling limits and the future development are discussed.
Keywords: LMB, Heat Transfer, Mass Transfer
  • Lecture (Conference)
    12th European Fluid Mechanics Conference, 09.-13.09.2018, Wien, Österreich

Permalink: https://www.hzdr.de/publications/Publ-27258
Publ.-Id: 27258


Machbarkeitsstudie zur Integration eines offenen MR-Scanners in die horizontale Strahlführung einer Protonentherapie-Anlage

Schellhammer, S. M.ORC; Karsch, L.; Smeets, J.; Pawelke, J.; Hoffmann, A. L.
Einleitung
Aufgrund der steilen Dosisgradienten kann die Treffgenauigkeit in der Protonentherapie (PT) durch Bewegungen und anatomische Veränderungen stark kompromittiert werden. Eine gleichzeitige Bildgebung mittels Echtzeit-Magnetresonanztomographie (MRT) könnte die Treffgenauigkeit erhöhen. Bis heute existieren jedoch keine kombinierten Systeme aus MRT und PT. Ziele dieser Studie waren deshalb die erste Integration eines MR-Scanners in eine PT-Strahlführung, die Überprüfung der Machbarkeit einer gleichzeitigen MR-Bildgebung und Bestrahlung, und die Kontrolle der MR-Bildqualität mit und ohne Strahleinfluss.

Material & Methoden
Ein offener MR-Scanner für muskuloskelettale Bildgebung mit einem vertikalen Magnetfeld von 0.22 T (MRJ2200, Paramed) wurde an einer strahldüsenlosen horizontalen Strahlführung (IBA Proton Therapy) installiert, und durch einen kompakten Faraday-Käfig von Hochfrequenz-Interferenzen abgeschirmt. Um den Protonenstrahl trotz der Strahlablenkung im Magnetfeld des Scanners zentral auf dessen Field-of-View zu richten, wurde das Magnetfeld mit einer Hall-Sonde (HHP-VU, Arepoc) vermessen. Auf dieser Grundlage wurde die mittlere Strahlablenkung für Energien zwischen 70−230 MeV mittels Monte-Carlo-Simulationen (Geant4) berechnet und der Scanner daraufhin um 2 cm versetzt zum Strahlaustritt platziert. Der Strahl wurde kollimiert (Ø=10 mm) und durch ein Strahlrohr in den Faraday-Käfig geführt. Die Strahllage im Field-of-View wurde mittels radiochromischer Filme (EBT3, Ashland) verifiziert. Zur Überprüfung der MR-Bildgebung wurden anatomische MR-Bilder eines Probanden bei deaktivierter Strahlführung sowie MR-Bilder eines Gewebephantoms mit und ohne Strahleinfluss (215 MeV, 5 nA) aufgenommen.

Ergebnisse
Die MR-Aufnahmen (Abb. 1) des Probanden zeigten die für den verwendeten Scanner übliche Bildqualität. Relevante anatomische Strukturen waren klar unterscheidbar. Am Gewebephantom wurde keine Bildverzerrung durch die Strahlführungsmagneten und den Protonenstrahl beobachtet, jedoch eine gleichförmige Bildverschiebung (< 1 mm) in Frequenzkodierrichtung, die vermutlich entweder auf statistische Schwankungen in der scannereigenen Frequenzkalibrierung oder auf das Randfeld der Strahlführungsmagnete zurückzuführen ist.

Zusammenfassung
Die Integration eines offenen MR-Scanners in den experimentellen Strahlengang einer Protonentherapie-Anlage war erfolgreich. Eine gleichzeitige MR-Bildgebung und Bestrahlung ohne Bildverzerrung ist möglich. Eine geringe und potentiell korrigierbare MR-Bildverschiebung wurde festgestellt.
  • Lecture (Conference)
    49. Jahrestagung der Deutschen Gesellschaft für Medizinische Physik, 19.-22.09.2018, Nürnberg, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-27257
Publ.-Id: 27257


THEREDA, the thermodynamic reference database for a nuclear waste disposal in Germany

Bok, F.; Moog, H. C.; Altmaier, M.; Voigt, W.; Thoenen, T.
The disposal of nuclear waste including the assessment of long-term safety is still an open question in Germany. In addition to the still pending decision about the repository host rock (salt, granite, or clay) the basic necessity of a consistent and obligatory thermodynamic reference database persists. Specific challenges are comprehensive datasets covering high temperatures and salinities. In response to deficiencies of other databases THEREDA, a joint project of institutions leading in the field of safety research for nuclear waste disposal in Germany and Switzerland, was started in 2006.
The core of THEREDA consists of a relational databank whose structure has been designed in a way that promotes the internal consistency of thermodynamic data. Data considered cover the needs of Gibbs Energy Minimizers and Law-of-Mass-Action programs alike. Pitzer coefficients to describe solute activity coefficients in high-saline solutions are considered. Both thermodynamic data and interaction coefficients can be described by temperature functions.
Ready-to-use parameter files are created from the databank in a variety of formats. Supported target codes are ChemApp, PHREEQC, EQ3/6, and Geochemist’s Work-bench. Data can alos be downloaded in a generic JSON-type format to promote conversion for other geochemical codes Prior to their release all parameter files are submitted to internal test calculations – one essential element of the quality assurance scheme. The results are documented and provided to the users and accessible via internet through http://www.thereda.de/.
Data are currently available to describe the solubility of the following radionuclides or fission elements: U(IV/VI), Th(IV), Np(IV/V), Pu(IV) Am(III), Nd(III), Cm(III), Tc(IV/ VII), Sr, Cs and the matrix elements (oceanic salt system, cement phases).
Future develpoments are thermodynamic data sets for Selenium and Oxygen in high saline solutions as well as the inclusion of low saline sorption data.
Keywords: THEREDA, Database, Thermodynamic Modelling, Radionuclides
  • Poster
    Goldschmidt2018, 12.-17.08.2018, Boston, USA

Permalink: https://www.hzdr.de/publications/Publ-27256
Publ.-Id: 27256


Thermodynamic modelling of Selenium in environmental conditions: traps, pitfalls and perspectives

Bok, F.; Jordan, N.; Brendler, V.
Any safety assessment of nuclear waste disposal concepts requires comprehensive and consistent thermodynamic data for the respective reactive transport modelling. This includes sorption, ion exchange or surface precipitation as major retardation processes, as well as a correct description of the aqueous chemistry including redox processes.
Selenium (with the isotope Se-79 being an important fission product) can occur in oxidation states varying between +VI and –II, the latter also including several polynuclear species. Most often negatively charged species are formed rendering them extraordinarily mobile in groundwater systems. Namely for Se solubility in highly saline solutions and for Se sorption onto minerals several competing thermodynamic datasets are published to predict the behavior of selenium under environmental conditions. However, there are still critical data gaps. For example, recent findings like the selenite dimerization have to be parameterized and included into thermodynamic data collections. In addition, for the selenide chemistry, solubility data are missing as well as ion-ion interaction parameters for the calculation in brines.
Another aspect of the reactive transport of selenium is the retardation of mainly selenate and selenite via sorption onto mineral phases. For these processes, recent spectroscopic investigations in combination with batch experiments have enabled deeper insights into the sorption chemistry of selenium. Here, the various data received must be processed into consistent data sets.
Several approaches to close critical selenium data gaps will be presented. These are essential steps towards a consistent and quality approved thermodynamic data set that can be included into databases needed for the geochemical and reactive transport calculations, namely THEREDA (http://www.thereda.de) and RES³T (http://www.hzdr.de/res3t).
Keywords: Radionuclides, Selenium, Thermodynamic Modelling, Databases
  • Lecture (Conference)
    256th ACS National Meeting & Exposition, 19.-23.08.2018, Boston, USA

Permalink: https://www.hzdr.de/publications/Publ-27255
Publ.-Id: 27255


Tailored Fano resonance and localized electromagnetic field enhancement in Ag gratings

Li, Z.; Klopf, J. M.; Wang, L.; Yang, K.; Lukaszew, R. A.
Metallic gratings can support Fano resonances when illuminated with EM radiation, and their characteristic reflectivity versus incident angle lineshape can be greatly affected by the surrounding dielectric environment and the grating geometry. By using conformal oblique incidence thin film deposition onto an optical grating substrate, it is possible to increase the grating amplitude due to shadowing effects, thereby enabling tailoring of the damping processes and electromagnetic field couplings of the Fano resonances, hence optimizing the associated localized electric field intensity. To investigate these effects we compare the optical reflectivity under resonance excitation in samples prepared by oblique angle deposition (OAD) and under normal deposition (ND) onto the same patterned surfaces. We observe that by applying OAD method, the sample exhibits a deeper and narrower reflectivity dip at resonance than that obtained under ND. This can be explained in terms of a lower damping of Fano resonance on obliquely deposited sample and leads to a stronger localized electric field. This approach opens a fabrication path for applications where tailoring the electromagnetic field induced by Fano resonance can improve the figure of merit of specific device characteristics, e.g. quantum efficiency (QE) in grating-based metallic photocathodes.

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Permalink: https://www.hzdr.de/publications/Publ-27254
Publ.-Id: 27254


U(VI) sorption by Ca-bentonite at pH 8-13: Spectroscopic investigation of retention mechanisms

Philipp, T.; Schmeide, K.; Rossberg, A.; Stumpf, T.
Bentonite is considered as buffer and backfill material in deep geological repositories for radioactive waste. Therefore, profound understanding of radionuclide retention processes at the bentonite surface under environmentally relevant conditions is essential for a long-term safety assessment. Such conditions can involve high pH, as hyperalkaline cement pore waters evolve from corroding concrete within a repository. Since the U(VI) sorption behavior at alkaline conditions is still poorly understood, batch experiments were combined with spectroscopic investigations in order to gain insight into the underlying retention processes on the molecular level.
pH-dependent batch sorption experiments (pH 8-13) in a diluted Gipshut solution (2.5 M NaCl, 0.02 M CaCl2, 0.02 M Na2SO4, 0.0051 M KCl) at different carbonate concentrations (absence, 0.5 and 100 mM) showed a decreased U(VI) retention in the presence of carbonate up until a certain pH (pH 9.5 or pH 11, depending on [CO32-]) due to the formation of weakly sorbing (calcium) uranyl carbonate complexes in aqueous solution, confirmed by time-resolved laser-induced fluorescence spectroscopy (TRLFS). This is in accordance with previous studies [1]. However, also in the presence of carbonate, U(VI) retention is increased in even stronger alkaline solutions, which is attributed to the preferred formation of hydrolyzed U(VI) species at these conditions.
In order to clarify the mechanisms responsible for the very strong U(VI) retention in the pH range 10-12 (absence and 0.5 mM CO32-), uranyl complexes on the bentonite surface were examined directly, using site-selective TRLFS and EXAFS (ESRF, Grenoble). Selective excitation of different sorption species by varying laser energy allowed the identification of both, surface complexation and, to a smaller degree, surface precipitation. EXAFS spectra did not show any indication of precipitates, verifying that adsorption is the dominant retention process and precipitates form only as small fractions, below the EXAFS detection limit. According to atomic distances and coordination numbers for U-Oeq, U(VI) surface complexes shift from a 5-fold to a 4-fold coordination in the equatorial plane with increasing pH.
  • Lecture (Conference)
    Goldschmidt2018, 12.-17.08.2018, Boston, USA

Permalink: https://www.hzdr.de/publications/Publ-27253
Publ.-Id: 27253


Data for "Complexation of trivalent lanthanides (Eu) and actinides (Cm) with aqueous phosphates at elevated temperatures"

Jordan, N.ORC; Starke, S.; Huittinen, N.ORC

At the Institute of Resource Ecology, the complexation of Eu(III) and Cm(III) with aqueous phosphate was studied using laser-induced luminescence spectroscopy at low pH ([H+] = 0.1 M), different ionic strengths (0.6 to 3.1 M) and different temperatures (25 to 80 °C). The data set contains the species distribution, slope analysis and the extrapolation to zero ionic strength using R.

Keywords: Curium; Europium; phosphate complexation; linear regression
  • Reseach data in the HZDR data repository RODARE
    Publication date: 2018-05-22
    DOI: 10.14278/rodare.5
    License: CC-BY-4.0

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Permalink: https://www.hzdr.de/publications/Publ-27252
Publ.-Id: 27252


CMOS‐compatible controlled hyperdoping of silicon nanowires

Berencén, Y.; Prucnal, S.; Möller, W.; Hübner, R.; Rebohle, L.; Böttger, R.; Glaser, M.; Schönherr, T.; Yuan, Y.; Wang, M.; Georgiev, Y. M.; Erbe, A.; Lugstein, A.; Helm, M.; Zhou, S.; Skorupa, W.
Hyperdoping consists of the intentional introduction of deep‐level dopants into a semiconductor in excess of equilibrium concentrations. This causes a broadening of dopant energy levels into an intermediate band between the valence and the conduction bands. Recently, bulk Si hyperdoped with chalcogens or transition metals is demonstrated to be an appropriate intermediate‐band material for Si‐based short‐wavelength infrared photodetectors. Intermediate‐band nanowires can potentially be used instead of bulk materials to overcome the Shockley–Queisser limit and to improve efficiency in solar cells, but fundamental scientific questions in hyperdoping Si nanowires require experimental verification. The development of a method for obtaining controlled hyperdoping levels at the nanoscale concomitant with the electrical activation of dopants is, therefore, vital to understanding these issues. Here, this paper shows a complementary metal‐oxide‐semiconductor (CMOS)‐compatible technique based on nonequilibrium processing for the controlled doping of Si at the nanoscale with dopant concentrations several orders of magnitude greater than the equilibrium solid solubility. Through the nanoscale spatially controlled implantation of dopants, and a bottom‐up template‐assisted solid phase recrystallization of the nanowires with the use of millisecond‐flash lamp annealing, Se‐hyperdoped Si/SiO2 core/shell nanowires are formed that have a room‐temperature sub‐bandgap optoelectronic photoresponse when configured as a photoconductor device.
Keywords: Flash lamp annealing, hyperdoping, intermediate band, ion implantation, nanowires

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Permalink: https://www.hzdr.de/publications/Publ-27251
Publ.-Id: 27251


Interaction of U(VI) with α-isosaccharinic acid under acidic conditions: characterization of the formed complexes

Brinkmann, H.; Patzschke, M.; Roßberg, A.; Moll, H.; Stumpf, T.
Cellulose is a very common organic polymer and also present in considerable amounts in low and intermediate level wastes (LILW). Since it is considered to stabilize LILW with cementitious materials and to use cement-based materials as construction and backfilling material, the alkaline degradation of cellulosic material has to be taken into account. This process will lead to the formation of water-soluble carboxylates and hydroxycarboxylates, with isosaccharinic acid (isa) being the main degradation product. It was shown that the α-form of the polyhydroxy-carboxylic acid is a stronger complexant compared to the β-form and that the interaction with radionuclides affects the solubility and the sorption behavior adversely [1]. Only a limited number of studies focused on the interaction of isa with UO22+. Hence, there are gaps in thermodynamic databases for this system. The basis for reliable thermodynamic data is a detailed structural knowledge about the formed species in the system of interest.

This issue prompted us to characterize the formed complexes in the UO22+-isa system on a molecular level. Our approach to elucidate the mechanisms in aqueous solution combines different spectroscopic techniques (UV-vis, ATR-FTIR, EXAFS, and luminescence) with DFT-calculations. The mutual influence of UO22+ and isa on their speciation as well as the three detected complexes will be discussed. The outcomes are on the one hand the basis for thermodynamic investigations as well as for studies under neutral and alkaline conditions. They provide on the other hand also important information concerning the behavior of α-isa as ligand, including dominant binding motifs.

[1] Van Loon, L. R., et al., Radiochimica Acta, 1999, Vol. 86, https://doi.org/10.1524/ract.1999.86.34.183.

This project has received funding from the Euratom research and training programme 2014-2018 under Grant Agreement no. 61880.
Keywords: uranium, isosaccharinic acid, spectroscopy, speciation
  • Lecture (Conference)
    18th Radiochemical Conference, 13.-18.05.2018, Mariánské Lázně, Czech Republic

Permalink: https://www.hzdr.de/publications/Publ-27250
Publ.-Id: 27250


Binding of Antimony to Natural Organic Matter in a Finish Mine-Water Influenced Peatland

Besold, J.; Eberle, A.; Kujala, K.; Kumar, N.; Scheinost, A. C.; Pacheco, L.; Fendorf, S.; Planer-Friedrich, B.
Antimony (Sb) is a toxic element typically of low natural abundance but human activities have led to highly elevated concentrations in many soils and sediments. Recently, natural organic matter (NOM) has been discussed as effective sink for arsenic [1] and first spectroscopic studies [2,3] indicated that sulfhydryl moieties of NOM also play an important role in controlling Sb mobility in wetland sediments. However, Sb speciation in NOM-rich wetlands has not yet been studied comprehensively and direct spectroscopic evidence for this sequestration mechanism is still lacking. In order to investigate the role of NOM for Sb sequestration, we used bulk Sb K-edge X-ray absorption fine structure spectroscopy (EXAFS) from a peatland in northern Finland which receives high Sb loads from an adjacent gold mine. Sampled peat cores were kept under argon atmosphere at cool and dark conditions until freeze-drying to prevent Sb speciation changes. The peat contained up to 52 % carbon and 265 mg/kg Sb (dry weight basis). Sulfur and iron contents ranged between 4 to 8 and 2 to 10 g/kg, respectively. Aqueous Sb concentrations decreased with lateral distance from the inflow from 190 µg/L in surface waters to 8 µg/L in 80 cm depth. Based on linear combination fitting of EXAFS spectra, we found Sb to be mainly coordinated to NOM moieties in all peat samples. At 10-20 cm depth, Sb was sorbed up to 47% to iron (hydr)oxides and with increasing depth, up to 50% of trivalent Sb was complexed tri-fold to sulfhydryl moieties of NOM. At these deep peat layers, Sb was up to 100% complexed to NOM. Our results show that sorption of Sb to particulate NOM can act as an important sequestration mechanism under sulfate reducing conditions and therefore strongly influences Sb mobility in the environment.

[1] Langner et al. (2012) Nat. Geosci. 5, 66-73. [2] Benett et al. (2017) Environ. Chem. 2017, 14, 345–349. [3] Arsic et al. (2018) Environ. Sci. Technol. 52, 1118-1127.
Keywords: antimony arsenic peat organic matter EXAFS XANES
  • Lecture (Conference)
    Goldschmidt Conference 2018, 12.-17.08.2018, Boston, U.S.A.

Permalink: https://www.hzdr.de/publications/Publ-27249
Publ.-Id: 27249


Core-Shell Structuring of Pure Metallic Aerogels towards Highly Efficient Platinum Utilization for the Oxygen Reduction Reaction - Kern-Schale-Strukturierung rein metallischer Aerogele für eine hocheffiziente Nutzung von Platin für die Sauerstoffreduktion

Cai, B.; Hübner, R.; Sasaki, K.; Zhang, Y.; Su, D.; Ziegler, C.; Vukmirovic, M. B.; Rellinghaus, B.; Adzic, R. R.; Eychmüller, A.
The development of core-shell structures remains a fundamental challenge for pure metallic aerogels. Here we report the synthesis of PdxAu-Pt core-shell aerogels composed of an ultrathin Pt shell and a composition-tunable PdxAu alloy core. The universality of this strategy ensures the extension of core compositions to Pd transition-metal alloys. The core-shell aerogels exhibited largely improved Pt utilization efficiencies for the oxygen reduction reaction and their activities show a volcano-type relationship as a function of the lattice parameter of the core substrate. The maximum mass and specific activities are 5.25 A mgPt-1 and 2.53 mA cm-2, which are 18.7 and 4.1 times higher than those of Pt/C, respectively, demonstrating the superiority of the core-shell metallic aerogels. The proposed core-based activity descriptor provides a new possible strategy for the design of future core-shell electrocatalysts.
Die Entwicklung von rein metallischen Aerogelen mit Kern-Schale-Strukturen ist nach wie vor eine grundlegende Herausforderung. Hier stellen wir die Synthese von PdxAu-Pt-Kern-Schale-Aerogelen vor, welche aus einer ultradünnen Pt-Schale und einem Kern aus einer PdxAu-Legierung mit einstellbarer Zusammensetzung bestehen. Die universelle Synthesestrategie ermöglicht eine Erweiterung der Kern-Zusammensetzung hin zu Pd-Übergangsmetall-Legierungen. Die Kern-Schale-Aerogele zeigen eine stark verbesserte Nutzungseffizienz von Pt in der Sauerstoffreduktion und ihre Aktivitäten folgen einem vulkanförmigen Verlauf bezüglich der Gitterparameter des Kern-Substrats. Mit einer maximalen massenbezogenen bzw. spezifischen Aktivität von 5.25 A mgPt-1 und 2.53 mA cm-2, welche 18.7- bzw. 4.1-mal höher sind als die für Pt/C, zeigt sich die Überlegenheit dieser metallischen Kern-Schale-Aerogele. Die vorgeschlagene kernbasierte Aktivitätsabhängigkeit liefert eine neue mögliche Strategie für den Entwurf zukünftiger Kern-Schale-Elektrokatalysatoren.
Keywords: aerogels, electrocatalysis, core-shell structures, oxygen reduction reaction, sol-gel processes - Aerogele, Elektrokatalyse, Kern-Schale-Strukturen, Nanostrukturen, Sol-Gel-Prozess

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Permalink: https://www.hzdr.de/publications/Publ-27248
Publ.-Id: 27248


The analysis of nothing and nearly nothing – concepts for reference materials for the Super-SIMS

Renno, A. D.ORC
The Super-SIMS idea goes back to the year 1979 [1]. Since then several attempts have been made to install such instruments [2-5], although with varied success.
Most of the published data were either analysis of semiconductor materials or isotope ratios of natural materials. Having a strong focus on natural, metal, and mineral resources the Helmholtz Institute Freiberg for Resource Technology installed such a system at the Ion Beam Centre at HZDR. This new Super-SIMS will be embedded into a system of consecutive micro-analytical methods devoted to the characterization of minerals and ores. Therefore, our focus will lie on the analysis of ultra-trace elements in these natural matrices.
Despite the high precision, the accuracy of SIMS analysis can be problematic. The sensitivity factor as well as the instrumental mass fractionation vary with the chemical composition. This so-called matrix effect demands that the sample and the reference material (RM) should have exactly the same chemical composition and structure, this is difficult to achieve. Even trace elements and in the case of the Super-SIMS ultra-trace elements may affect the sensitivity factor. The compromise is the usage of matrix matched RMs.
The combination of good lateral and depth resolution of the SIMS instrument with the resulting small sample volumes / masses (sub ng-range) and the aspired detection limits in the pg/g range yield to the fact that the probability to meet one atom of the analyte in the sample volume will be < 1.
This contribution will stimulate the discussion about the concepts of detection limit, homogeneity and heterogeneity in RMs and present considerations about the design of future RMs for ultra-trace element analysis with the Super-SIMS.

[1] Purser et al. Surface and Interface Analysis 1(1), 1979, 12.; [2] S. Matteson, Mass Spectrom. Rev., 27 (2008) 470.; [3] Ender et al. NIMB 123 (1997) 575.; [4] Maden, PhD thesis, ETH Zurich 2003.; [5] Fahey et al. Analytical Chemistry 88(14), 2016, 7145
Keywords: Reference Materials, SIMS, Super-SIMS
  • Poster
    Geoanalysis 2018, 08.-13.07.2018, Sydney, Australia

Permalink: https://www.hzdr.de/publications/Publ-27247
Publ.-Id: 27247


A Super-SIMS for resource technology

Renno, A. D.ORC; Akhmadaliev, S.; Belokonov, G.; Böttger, R.; von Borany, J.; Gutzmer, J.; Kaever, P.; Meyer, M.; Noga, P.; Rugel, G.; Tiessen, C. J.; Voigtländer, J.; Wagner, N.; Wiedenbeck, M.; Winter, A.; Wu, H.; Ziegenrücker, R.
The integration of an ion source with very high spatial resolution with a tandem accelerator is a long-standing concept for improving analytical selectivity and sensitivity by orders of magnitude [1-3]. Translating this design concept to reality has its challenges [e.g. 4-6]. Supporting a strong focus on natural, metallic and mineral resources the, Helmholtz Institute Freiberg for Resource Technology installed such a system at the Ion Beam Centre at HZDR. This so-called Super-SIMS will be at the core of a comprehensive pallet of micro-analytical methods devoted to the characterization of minerals and ores. Secondary ion beam from a CAMECA IMS 7f-auto are injected into the pre-existing 6MV Dresden Accelerator Mass Spectrometry facility [7,8], which quantitatively eliminates isobaric molecular species from the ion beam. Our SIMS component can function as either a stand-alone device or can be used to inject the negatively charged secondary ions at energies of up to 40 keV (to match the acceptance conditions) into the accelerator. A dedicated ion optical unit has been constructed and installed to match the SIMS ion beam to the maximum acceptance of the accelerator.
We will present measurements of the performance parameters of the instrument as well as first results of halogen (F, Cl, Br, and I) determinations in galena, sphalerite and pyrrhotite.
[1] Purser et al. Surface and Interface Analysis 1(1), 1979, 12. [2] J. M. Anthony, D. J. Donahue, A. J. T. Jull, MRS Proceedings 69 (1986) 311-316. [3] S. Matteson, Mass Spectrom. Rev., 27 (2008) 470. [4] Ender et al. NIMB 123 (1997) 575. [5] Maden, PhD thesis, ETH Zurich 2003. [6] Fahey et al. Analytical Chemistry 88(14), 2016, 7145. [7] Akhmadaliev et al., NIMB 294 (2013) 5. [8] Rugel et al. NIMB 370 (2016) 94.
Keywords: Super-SIMS, SIMS
  • Lecture (Conference)
    Geoanalysis 2018, 08.-13.07.2018, Sydney, Australia

Permalink: https://www.hzdr.de/publications/Publ-27246
Publ.-Id: 27246


Box-profile implants as geochemical reference materials for EMP and SIMS

Wu, H.; Belokonov, G.; Böttger, R.; Couffignal, F.; Munnik, F.; Renno, A. D.ORC; Wiedenbeck, M.; Ziegenrücker, R.
EMP (Electron Microprobe) and SIMS (Secondary Ion Mass Spectrometry) are widely used analytical techniques for geochemical and mineralogical applications. Nevertheless, metrologically rigorous quantification remains a major challenge for these methods. SIMS in particular is a matrix sensitive method; the use of matrix-matched reference materials (RMs) is essential in order to avoid significant analytical bias. A major problem is that the list of available reference materials for SIMS is vanishingly short compared to the needs of the analyst. A current evaluation of the GeoReM database [1] shows a strong focus on using the well-known NIST SRM 610-617 glasses for trace element analysis along with several zircons for isotope analysis, with few other matrices being readily available.
One approach for the production of matrix specific RMs is the use of ion implantation that introduces a known amount of a selected isotope into a material. This strategy is widely-used for SIMS applications in materials science, but rarely used for geochemical applications. Bumett et al. (2015) [2] demonstrated the appropriateness of this method. We choose the more elaborate way of implanting a so-called box profile to generate a homogeneous concentration of the selected isotope in three dimensions.
For proof of concept we used the mineralogically and chemically “simple” SiO2 system which addresses many interesting scientific challenges, such as the Ti-in-quartz geothermometer [3]. We implanted either 47Ti or 48Ti into synthetic, ultra-high purity silica glass. Several box profiles with concentrations between 10 and 1000 µg/g Ti and a maximum depth of homogeneous Ti distribution between 200 and 3000 nm were produced at the Ion Beam Center in Dresden-Rossendorf. Multiple implantation steps using differing ion energies and ion doses were simulated with the SRIM (Stopping and Range of Ions in Matter) software [4], optimizing for the target concentrations, implantation-depths and technical limits of the implanter. A thorough TEM assessment showed that the Ti is dispersed throughout the glass structure. We characterized several implanted test-samples by means of SIMS, EMP and other analytical techniques. The homogeneity of the Ti-concentration is within ± 5% uncertainty in all 3 dimensions.
[1] http://georem.mpch-mainz.gwdg.de, [2] D. S. Bumett, et al., Geostandards and Geoanalytical Research 39(3), 2015, 265-276., [3] J. B. Thomas, et al., Contrib. Mineral. Petr. 160(5), 2010, 743–759., [4] J. F. Ziegler, Nucl. Instrum. Meth. B 219-220, 2004, 1027-1036.
Keywords: Reference Materials, SIMS, EMP, Super-SIMS, implantation
  • Poster
    Geoanalysis 2018, 08.-13.07.2018, Sydney, Australia

Permalink: https://www.hzdr.de/publications/Publ-27245
Publ.-Id: 27245


Detecting and quantifying the relativistic Kelvin-Helmholtz instability in interstellar jets via radiation observable on Earth

Pausch, R.; Bussmann, M.; Huebl, A.; Schramm, U.; Steiniger, K.; Widera, R.; Debus, A.
We present a microscopic model of the radiation emitted during the relativistic Kelvin-Helmholtz instability (KHI) and validate our findings with particle-in-cell simulations at unprecedented spatial resolution and size that including complete far-field radiation spectra.

The KHI is expected in shear flow regions of astrophysical plasma jets, which are significant sites for particle acceleration and radiation. We demonstrate that the emitted polarized radiation can be used to identify and characterize the microscopic plasma dynamics of a KHI light-years away. We have simulated the radiation of the KHI using the particle-in-cell code PIConGPU. With this code's synthetic radiation diagnostic, based on Liénard-Wiechert potentials, quantitative predictions of the far field radiation for hundreds of observation directions and a frequency range covering 3 orders of magnitude were performed on the TITAN cluster at Oak Ridge National Laboratory. The simulation showed that the time-dependent changes in the radiation polarization and power correlate directly with the stages of the KHI. This allows identifying the linear growth phase of the KHI and quantifying its characteristic growth rate as predicted by our microscopic model.
Keywords: Kelvin Helmholtz instability, Particle-in-cell, PIConGPU, radiation
  • Lecture (Conference)
    DPG-Frühjahrstagung Würzburg, 19.-23.03.2018, Würzburg, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-27244
Publ.-Id: 27244


In-situ synthetic radiation diagnostics for laser wakefield acceleration

Pausch, R.; Debus, A.; Huebl, A.; Schramm, U.; Steiniger, K.; Widera, R.; Bussmann, M.
We present recent results of LWFA simulations including in-situ radiation diagnostics performed with the particle-in-cell code PIConGPU. Our results demonstrate the power provided by synthetic radiation diagnostics to determine the laser-plasma dynamics with regard to applications in experiments.

PIConGPU is currently one of the fastest 3D3V particle-in-cell codes and provides an in-situ radiation diagnostic based on Liénard-Wiechert potentials. This synthetic diagnostic is capable of quantitatively predicting the spectrally and directionally resolved far-field radiation of billions of macro-particles by an in-situ implementation in the PIC cycle. Among other things, the code enables resolving the spatial origin and temporal evolution of the radiation, determine the polarization, quantifying both coherent and incoherent radiation simultaneously and covering a frequency range from infrared to x-rays.

The talk briefly introduces the technical background of computing the radiation in-situ on GPUs. Its main focus, however, is the characteristic radiation of LWFA that allows identifying the various stages of the laser-plasma dynamics. Possible applications of these radiation signatures in laboratory experiments will be discussed.
Keywords: Laser Wakefield Accelerator, Particle-in-cell, radiation
  • Lecture (Conference)
    DPG-Frühjahrstagung Würzburg, 19.-23.03.2018, Würzburg, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-27243
Publ.-Id: 27243


The prognostic value of FMISO-PET-based synchronous tumor and lymph node hypoxia outperforms that of tumor hypoxia only in patients with advanced stage HNSSC – secondary analysis of Dresden FMISO trail

Bandurska-Luque, A.; Löck, S.; Haase, R.; Richter, C.; Zöphel, K.; Perrin, R.; Seidlitz, A.; Zschaeck, S.; Appold, S.; Krause, M.; Steinbach, J.; Kotzerke, J.; Zips, D.; Baumann, M.; Troost, E.
Purpose: Primary tumor (Tu) hypoxia based on hypoxia-PET is a known prognostic parameter for locally-advanced head-and-neck squamous cell carcinoma (HNSCC) patients. This secondary analysis of the prospective clinical trial [1] on repeat [18F]fluoromisonidazole (FMISO) PET/CT before and during radiochemotherapy (RCT) compared the prognostic value of synchronous Tu and lymph node metastases (LN) hypoxia with that of hypoxia only determined in Tu.

Methods: Forty-five LN-positive patients with 103 LNs were included in this analysis. FMISO-PETs were performed at baseline, week 1, 2 and 5 of RCT. Based on a qualitative scale, Tu and LN were independently categorized as hypoxic or normoxic, being FMISO uptake higher than or equal to background, respectively. Two prognostic parameters were defined: Tu-hypoxia (patients with a hypoxic Tu, independent of the LN oxygenation status) and synchronous Tu-and-LN-hypoxia. In fifteen patients with a large LN (n = 21) a quantitative analysis of FMISO PET was performed to validate hypoxia scale and to correlate with regional control (RC). Log-rank, uni- and multivariate Cox test were used to assess the parameters’ prognostic impact on locoregional control (LRC), RC and time to progression (TTP).

Results: Synchronous Tu-and-LN-hypoxia was a strong adverse prognostic factor for LRC and TTP at all time-points (p ≤ 0.005) whereas Tu-hypoxia only was significantly associated with poor LRC in week 2 and 5 (p ≤ 0.004) and with short TTP in week 1, 2 and 5 (p ≤ 0.043). The quantitative FMISO parameters correlated with RC. There was a significant correlation between the qualitative and quantitative FMISO parameters (R > 0.6–0.8).

Conclusions: FMISO-based synchronous hypoxia in the primary tumor and lymph node metastases holds strong prognostic information in HNSCC patients outperforming that based on primary tumor hypoxia only. Confirmation in ongoing prospective trials is intended before introducing in personalized radiation oncology.
  • Lecture (Conference)
    33. Deutscher Krebskongress 2018, 21.-24.02.2018, Berlin, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-27241
Publ.-Id: 27241


Dose-dependent changes after proton and photon irradiation in zebrafish model

Brunner, S.; Tőkés, T.; Szabó, E. R.; Szabó, I. Z.; Polanek, R.; Beyreuther, E.; Pawelke, J.; Hideghéty, K.
Purpose/Objective: The laser-driven ionizing (LDI) beams have unique property of ultra-high dose rate, ultra-short pulses and carry the potential toward special clinical application. Our aim was to establish an in vivo zebrafish model for radiobiological research on later LDI radiation.
Material/methods: 24 hours post-fertilization (hpf) zebrafish (Danio rerio) embryos were irradiated at the University Proton Therapy Dresden with escalated doses (5, 10, 15, 20 and 30 Gy) at two positions along the proton depth-dose curve, at the plateau and at the middle of Spread Out Bragg Peak, and with reference 6 MV photon beams from a clinical linac (n=96 in each group). The experiment was 3 times repeated under the same conditions. On the 3th (96 hpf) and 4th (120 hpf) days after irradiation morphological malformations were documented (photo) and determined quantitatively. Two independent observers measured the length of the embryos, the degree of the yolk sac edema and the diameter of the eyes. Additionally, we have detected the DNA double-strand breaks immunohistochemically (gamma-H2AX foci) after 30 min of the irradiation at the two positions of the proton (mSOBP and plateau) and photon beams, at 5 Gy dose level.
Results: Dose-dependent organ developmental deteriorations could be detected morphologically at >10 Gy dose levels. The length of the embryo and the size of the eyes reduced, while the yolk sac edema increased significantly in dose dependent degree after 10 Gy, 15 Gy, 20 Gy and 30 Gy irradiation, at both developmental stages. At 5 Gy dose irradiation we have found significant elevation in the number of DNA double-strand breaks, as compared to the unirradiated control groups. Furthermore, data showed that after proton irradiation the degree of the DNA damage was higher, as compared to the photon irradiation.
Conclusion: We could establish a reliable quantitative morphological analysis of dose-dependent organ malformations using an in vivo vertebrate system. The zebrafish embryo model proved to be appropriate for complex evaluation of the irradiation-caused damages, molecular changes and for comparison of the biological effects of different radiation qualities. We could define the optimal parameters for future radiobiological experiments with the LDI beams.
Supported by: The ELI-ALPS project (GINOP-2.3.6-15-2015-00001) is supported by the European Union and co-financed by the European Regional Development Fund. The project has received funding from the European Union's Horizon 2020 research and innovation programme under grant agreement no 654148 Laserlab-Europe and by the German BMBF, grant no. 03Z1N511.
  • Open Access Logo Abstract in refereed journal
    Radiotherapy and Oncology 127(2018)1, S588
    DOI: 10.1016/S0167-8140(18)31356-2
  • Poster
    37. ESTRO Meeting, 20.-24.04.2018, Barcelona, Spain

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Permalink: https://www.hzdr.de/publications/Publ-27240
Publ.-Id: 27240


Development of zebrafish embryo model for radiobiology research at ELI-ALPS on laser driven hadron beams

Szabó, E. R.; Tőkés, T.; Polanek, R.; Szabó, Z.; Brunner, S.; Czifrus, S.; Fenyvesi, A.; Biró, B.; Beyreuther, E.; Pawelke, J.; Hideghéty, K.
Purpose/objective: High power lasers provide the basis of particle acceleration, but at the actual status of the development, low energy, limited size beams with special properties (ultrahigh dose rate, pulsed mode) are available under technical conditions for radiobiology experiments. Our main aim was to introduce, optimize and validate a vertebrate system for in vivo experiments to study the biological effects of novel hadron beams.
Material/methods: Series of zebrafish embryos in different ages (from 1 hour post-fertilization (hpf) to 72 hpf), in different holders varying the number/well were prepared. For irradiation we used fission neutron (0, 1.25, 1.875, 2, 2.5 Gy), cyclotron-based neutron (0, 2, 4, 6.8, 8.12, 10.28 Gy) and proton (0, 5, 10, 15, 20 and 30 Gy) at two positions along the proton depth-dose curve (PDDC): at the plateau and at the middle of Spread Out Bragg Peak (mSOBP), furthermore, with reference linear accelerator photon (0, 5, 10, 15, 20 Gy) beam (n=96 in each group), repeated several times (≥3). Thereafter, survival, any type of organ developmental disturbance (pericardial edema, spine curvature, shortening of the body length and micro-opthalmia) were detected each days up to 7 post irradiation days (pid). Histological evaluation (size of the eye, brain necrosis, intestinal changes, liver vacuolization, hyper eosinophilic necrotic muscle-fibers) and molecular changes were evaluated with RT-PCR method at certain time points post irradiation.
Results: A higher vulnerability and radiation sensitivity could be observed at earlier stages of the embryogenesis (1-12 hpf). The LD50 was determined with the well reproducible survival curves, resulting in RBE between 10 and 4.8 for the 1MeV and 14MeV neutrons and the Relative Biological Effectivity (RBE) around 1.1-1.4 for proton sources at the two positions respectively. The morphological distortions shown close correlation to the dose delivered and their evaluation on the 4th pid exhibited a good agreement to the survival derived RBE. The gravity of the histopathological changes on the basis of semi-quantitative analysis corresponded well to the macro morphological abnormalities (eye layer disorganization, degree of brain necrosis, increased numbers of the goblet cells in the gastrointestinal tract, and muscle fibrosis).
Conclusion: Numerous features of the zebrafish embryo model makes it amenable for large scale of radiobiological investigations. On the basis of our experimental series the optimal embryonal age (hpf), radiation setup and observation time points for assessment of the different biological endpoints could be established. The defined parameters proved to be suitable for reliable RBE determination.

Acknowledgement: The ELI-ALPS project (GINOP-2.3.6-15-2015-00001) is supported by the European Union and co-financed by the European Regional Development Fund, and by the German BMBF, grant nos. 03ZIK445 and 03Z1N511. The project has received funding from the European Union's Horizon 2020 research and innovation program under grant agreement no 654148 Laserlab-Europe.
  • Poster
    37. ESTRO Meeting, 20.-24.04.2018, Barcelona, Spain
  • Open Access Logo Abstract in refereed journal
    Radiotherapy and Oncology 127(2018)Suppl1, S586
    DOI: 10.1016/S0167-8140(18)31353-7

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Permalink: https://www.hzdr.de/publications/Publ-27239
Publ.-Id: 27239


Hazard statements: looking for alternatives to toxicity evaluation using LCA

Rodriguez-Garcia, G.; Braun, J.; Peters, J.; Weil, M.
Life Cycle Assessment is a methodology for the evaluation of potential hazards to the environment and to human health. It can be used for decision support when selecting materials for a product. It is a detailed method that can become very labor intensive. As alternatives, we introduce here two methodologies for ranking products and materials according to their safety: Both methods are built on two pieces of European legislation. Hazard Traffic Lights is a qualitative visual way to quickly identify potential hazards. Total Hazard Points is a quantitative method for weighting the different hazards related to a product. It is based on the method developed for the German Environmental Agency (UBA), but its scope includes all materials and hazards, rather than a selection of them. As a case study, we evaluated the 9 batteries described in the UBA study and compared our results with those presented there. In our opinion, batteries are in general terms more hazardous in the UBA study. This is due to more thorough identification of hazards –including some potentially more significant – and the inclusion of all the potential hazards of a material. Since not all the materials present in the battery were quantified, both sets of results should be considered an underestimation of the possible hazard.

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Permalink: https://www.hzdr.de/publications/Publ-27237
Publ.-Id: 27237


AMS of 93 Zr: Passive absorber versus gas-filled magnet

Hain, K.ORC; Deneva, B.; Faestermann, T.; Fimiani, L.; Gómez-Guzmán, J. M.; Koll, D.; Korschinek, G.; Ludwig, P.; Sergeyeva, V.; Thiollay, N.
Two different isobar separation techniques were tested for the detection of the long-lived fission product 93Zr (T1/2T1/2 = 1.64 ·· 106 a) using Accelerator Mass Spectrometry (AMS), i.e. a passive absorber and a gas-filled magnet, respectively. Both techniques were used in combination with a Time-of-Flight path for the identification of the stable neighboring isotopes 92Zr and 94Zr. The passive absorber was represented by a stack of silicon nitride foils for high flexibility regarding the thickness for optimal isobar separation. Ion beams with a large variety of energies, between 80 and 180 MeV, were provided for this experiment by the tandem accelerator at the Maier-Leibnitz Laboratory in Garching, Germany. With these beams, the stopping powers of 93Zr and 93Nb as a function of energy were determined experimentally and compared to the results obtained with the simulation program SRIM. Considerable discrepancies regarding the energy dependence of the two stopping power curves relative to each other were found. The lowest detection limit for 93Zr achieved with the passive absorber setup was 93Zr/Zr = 1 ·· 10−10. In comparison, by optimizing the gas-filled magnet set-up, 93Nb was suppressed by around six orders of magnitude and a detection limit of 93Zr/Zr = 5 ·· 10−11 was obtained. To our knowledge, these results represent the lowest detection limit achieved for 93Zr until now.
Keywords: 93Zr; AMS; Gas-filled magnet; Passive absorber

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Permalink: https://www.hzdr.de/publications/Publ-27236
Publ.-Id: 27236


Bubbly Flow in Stirred Tanks: Euler-Euler / RANS Modeling

Shi, P.ORC; Rzehak, R.
Aerated stirred tanks are frequently used equipment in industries ranging from chemical engineering and biotechnology to minerals processing. In principle, CFD simulation of such equipment on industrial scales is feasible within the Euler-Euler framework of interpenetrating continua. Practical application, however, requires suitable closure models to account for phenomena on the scale of individual bubbles, which are not resolved in this approach. The present work applies a set of closure relations that was previously used with good success to describe bubbly flows in pipes and bubble columns. It turns out that model extensions are needed concerning turbulence and the drag force. To validate the model a comprehensive set of experimental data including gas fraction as well as liquid velocity and turbulence has been assembled from different literature sources. The finally proposed extended model compares reasonably well with this dataset.
Keywords: aerated stirred tanks, dispersed gas-liquid multiphase flow, Euler-Euler two-fluid model, closure relations, Reynolds-stress turbulence model, CFD simulation, model validation

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Permalink: https://www.hzdr.de/publications/Publ-27235
Publ.-Id: 27235


Integrating a low-field open MR scanner with a static proton therapy research beamline: proof of concept

Schellhammer, S. M.ORC; Karsch, L.; Smeets, J.; Pawelke, J.; Hoffmann, A. L.
Purpose
On-line image guidance using magnetic resonance (MR) imaging is expected to improve targeting precision in proton therapy (PT). However, to date no hybrid MR-PT system exists. This is partly due to unknown mutual electromagnetic interactions between the MR scanner and the PT beamline, which may compromise the quality of the proton beam or the MR image. The aim of our study was to integrate an MR scanner with a static PT research beamline and to test the feasibility of simultaneous irradiation and imaging.

Materials & methods
An open MR scanner (MrJ2200, Paramed) featuring a 0.22 T vertical permanent magnetic (B0) field was RF-shielded by a compact Faraday cage and placed at the beam exit of a horizontal static PT research beamline (IBA Proton Therapy). To account for Lorentz force-induced beam deflection in B0, the scanner had to be laterally displaced by 2 cm from the beam’s central axis, such that a proper co-alignment of the beam and the scanner’s field-of-view (FOV) could be confirmed by radiochromic film (Gafchromic EBT3, Ashland) measurements. The beam was collimated to Ø10 mm before entering the Faraday cage through a cylindrical beam guide (Fig. 1).

MR test: With the beamline magnets off, the knee, wrist and hip of a volunteer were scanned with STIR gradient echo (GE), T1-weighted GE, and T1-weighted spin echo (SE) imaging, respectively. T1-weighted SE images of a mixed-meat sausage were acquired using a knee coil without beam, with beamline magnets on and while being irradiated at 215 MeV and 5 nA for 5 minutes.

Beam test: With Faraday cage removed, beam profiles were acquired with and without MR scanner for 72, 125 and 219 MeV beams using a pixelated scintillation detector (Lynx, IBA Dosimetry) positioned 110 cm downstream of the MR scanner's isocentre. These measurements were repeated with the MR scanner in place during acquisition of three different SE and GE images (max. gradient strength up to 5.7 mT/m).

Results
MR test: MR imaging in the nearby presence of a PT beamline was feasible and showed sufficient quality for anatomical imaging of human musculoskeletal structures. MR images of the meat sausage acquired with operating beamline showed a uniform translation of <2 mm in frequency encoding direction, but no geometrical distortions.

Beam test: The scintillation detector showed a horizontal beam deflection of 22, 16 and 11 cm for 72, 125 and 219 MeV, respectively, and a vertical beam deflection <0.6 mm. Horizontal deflection was taken into account to install an in-cage beam stopper, while vertical deflection could be neglected. The beam profiles showed no influence of the gradient fields applied during image acquisition.

Conclusions
For the first time, the integration of an MR scanner and a static PT research beamline has been realized. By taking into account the scanner’s B0 field induced beam deflection, simultaneous proton beam irradiation and MR imaging of an object placed in the scanner’s FOV was feasible with acceptable beam and image quality. The beamline-induced MR image shift is subject of an ongoing performance evaluation study.
  • Lecture (Conference)
    MR in RT symposium, 30.06.-03.07.2018, Utrecht, Nederland

Permalink: https://www.hzdr.de/publications/Publ-27234
Publ.-Id: 27234


Commissioning of a 4D dynamic MRI motion phantom on a 3T MR scanner: motion validation study

Schneider, S.; Dolde, K.; Engler, J.; Hoffmann, A.; Pfaffenberger, A.
Purpose:
Systems for integrated magnetic resonance guided radiation therapy (MRgRT) provide real-time and on-line MRI guidance for unequalled targeting performance of moving tumours and organs at risk. The clinical introduction of such systems requires dedicated methods for commissioning, routine machine quality assurance (QA) and verification of gated and adaptive treatment plans. The aim of the study was to develop a commissioning protocol and method for automatic quantification of target motion and geometrical fidelity using a 4D dynamic MRI motion phantom.

Materials & Methods:
The CIRS MRI-LINAC Dynamic Phantom (Model 008M) was positioned on a flat tabletop overlay (Medibord Ltd) in a 3.0T MR scanner (Ingenuity TF PET/MR, Philips) using an in-house constructed base plate for a quick and reproducible setup. The torso-shaped phantom body, which was filled with mineral oil (Marcol Blend, Philips), includes a 3D grid structure for image distortion analysis and a cylindrical thru-hole in which a software-controlled moving rod with a hypo-intense background gel and a decentralized hyper-intense target simulates 3D organ motion patterns. The geometric image distortion was determined as the mean and maximum Euclidean distance (∆mean, ∆max) between grid points in 3D spoiled gradient echo (THRIVE) MRI- and CT scans (Siemens Somatom Definition AS) after registration by means of the central fiducial. Sinusoidal 1D/2D/3D and a volunteer navigator scan-based 1D target motion pattern were evaluated using 2D cine MRI balanced turbo field echo sequences at a temporal resolution of 1.5-2 Hz. The motion tracking was performed with different pre-set frequencies (0.1-0.2 Hz) and amplitudes (up to 40/10/10 mm in IS/AP/LR direction). The target’s centre-of-mass motion pattern was reconstructed by an in-house developed automated image tracking algorithm implemented in MATLAB.

Results:
The base plate enabled a reproducible setup with a deviation of <1 mm in all directions. The geometric distortion increased with distance from the phantom’s centre predominantly in anterior direction, with ∆mean=0.56+/-0.28 mm and ∆max=1.5 mm in the THRIVE sequence relative to the CT scan. The frequencies of the reconstructed motion patterns from 2D cine MRI agree to the pre-set values within 2%; the reconstructed amplitudes showed a maximum deviation to the pre-set amplitudes of <0.8 mm in AP/LR direction and <0.4 mm in IS direction.

Conclusions:
A method and protocol for commissioning a 4D MRI dynamic motion phantom on a 3.0T MR scanner for MRgRT was developed. High-contrast and geometrically reliable 2D cine MR images of the phantom’s moving target could be obtained. The pre-set motion parameters could be extracted with sufficient spatio-temporal accuracy from 2D cine MRI in all motion directions. The method developed can be used for routine QA tests of spatio-temporally resolved MRI data in MRgRT.
Keywords: Phantom, Motion, MRI
  • Lecture (Conference)
    6th MR in RT Symposium 2018, 30.06.-03.07.2018, Utrecht, Niederlande

Permalink: https://www.hzdr.de/publications/Publ-27233
Publ.-Id: 27233


„Radiobiology of Proton Therapy“: results of an international expert workshop

Lühr, A.; von Neubeck, C.; Pawelke, J.; Seidlitz, A.; Peitzsch, C.; Bentzen, S.; Bortfeld, T.; Debus, J.; Deutsch, E.; Langendijk, J.; Löffler, J.; Mohan, R.; Scholz, M.; Sørensen, B.; Weber, D.; Baumann, M.; Krause, M.
The physical properties of proton beams offer the potential to reduce toxicity in tumor-adjacent normal tissues. Towards this end, the number of proton radiotherapy facilities has steeply increased over the last 10-15 years to currently around 70 operational centers worldwide. However, taking full advantage of the opportunities offered by proton radiation for clinical radiotherapy requires a better understanding of the radiobiological effects of protons alone or combined with drugs or immunotherapy on normal tissues and tumors. This report summarizes the main results of the international expert workshop “Radiobiology of Proton Therapy” that was held in November 2016 in Dresden.
It addresses the major topics (1) relative biological effectiveness (RBE) in proton beam therapy, (2) interaction of proton radiobiology with radiation physics in current treatment planning, (3) biological effects in proton therapy combined with systemic treatments, and (4) testing biological effects of protons in clinical trials.
Finally, important research avenues for improvement of proton radiotherapy based on radiobiological knowledge are identified. The clinical distribution of radiobiological effectiveness of protons alone or in combination with systemic chemo- or immunotherapies as well as patient stratification based on biomarker expressions are key to reach the full potential of proton beam therapy. Dedicated preclinical experiments, innovative clinical trial designs, and large high-quality data repositories will be most important to achieve this goal.
Keywords: proton therapy, relative biological effectiveness, RBE, LET, radiobiology, clinical trials

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Permalink: https://www.hzdr.de/publications/Publ-27232
Publ.-Id: 27232


Integrating a low-field open MR scanner with a static proton therapy research beamline: Characterisation of in-beam imaging performance

Gantz, S.; Schellhammer, S. M.; Grossinger, P.; Karsch, L.; Smeets, J.; Serra, A.; Pawelke, J.; Hoffmann, A. L.
Purpose
For the successful integration of MRI and proton therapy (PT), the mutual electromagnetic interaction between both systems needs to be investigated. So far, no combined system existed to investigate the MR imaging performance in the presence of a proton beam. Here, the aim is to characterize the imaging performance of a first in-beam MRI scanner during simultaneous proton irradiation and imaging.

Materials & methods
A 0.22 T open MRI scanner (MrJ2200, Paramed) has been installed at the horizontal static research beamline of our PT facility. The imaging performance characterization included both magnetic field homogeneity (MFH) measurements and ACR phantom tests for image quality. The MFH was mapped over a 22 cm diameter spherical volume by a magnetic field camera (MFC3045/48, Metrolab) being placed in the centre of the scanner’s field-of-view (FOV). To assess the effect of magnetic fringe fields of the nearby beamline magnets, the MFH was measured without and with magnets energized for beam energies between 70220 MeV. Phantom imaging tests were performed with the ACR small phantom being centrally positioned in the scanner FOV inside a knee coil (Fig. 1). Images were acquired by performing T1- and T2-weighted spin echo (SE) sequences with parameter settings according to the ACR phantom test protocol. Additionally, T1 and T2*- weighted gradient echo (GES and GEL, respectively) scans were performed. The phantom was irradiated by a 125 MeV pencil beam (Ø=10 mm) at dose rates of 1 and 80 Gy/min. Images were acquired for six different scenarios, starting from a reference scan with beamline magnets and beam off, followed by sequentially switching on first the beamline magnets and then the beam during both radiofrequency calibration and image acquisition or during image acquisition alone. A validated software tool (MATLAB) was used to extract the ACR imaging parameters and to estimate geometric transformations from image pairs acquired for the different scenarios.

Results
The peak-to-peak MFH was 88 ppm, which is within the scanner’s operating specifications. The MFH measurements with and without energized beamline magnets showed no significant differences (<3 ppm), but the mean baseline resonance frequency was increased by 70110 Hz depending on beam energy. The SE and GEL image quality was sufficient for analysis. GES images showed a low SNR (<15) and suffered from banding artefacts, which prevented automated evaluation of ACR parameters. For all six scenarios, differences in ACR parameters were within measurement uncertainties. A sequence-dependent uniform image translation of 0.53.0 mm in frequency encoding direction was observed due to operating the beamline. These image translations were in accordance with the baseline resonance frequency shift and showed to be inversely proportional to the gradient strengths of the sequences used (0.75.7 mT/m).

Conclusion
The imaging performance of a first low-field in-beam MRI scanner integrated with a static PT research beamline meets vendor and ACR image quality specifications. No degradation of the imaging performance was observed during simultaneous operation of the MRI and PT systems. Beamline induced off-resonance image translations need to be compensated for in the different imaging sequences.
  • Lecture (Conference)
    MR in RT Symposium, 30.06.2018, Utrecht, Niederlande

Permalink: https://www.hzdr.de/publications/Publ-27231
Publ.-Id: 27231


Marangoni convection at electrogenerated hydrogen bubbles

Yang, X.ORC; Baczyzmalski, D.; Cierpk, C.; Mutschke, G.; Eckert, K.ORC
Electrolytic gas evolution is a fundamental phenomenon occurring in a large number of industrial applications. In these processes gas bubbles are formed at the electrode from a supersaturated solution. Since dissolved gases can change the surface tension, a gas concentration gradient may cause the surface tension to vary locally at the gas bubble. Surface tension gradients may also form due to temperature gradients generated by ohmic heating of the electrolyte. In both cases, the resulting shear stress can impose a convection in the electrolyte and the gas bubble (Marangoni effect). This phenomenon may influence the entire electrolytic gas evolution process, e.g., by an enhanced mass transfer. In this study, the first evidence of the Marangoni convection near growing hydrogen bubbles, generated by water electrolysis, is provided. Microscopic high speed imaging was applied to study the evolution of single hydrogen bubbles at a microelectrode.
The convection near the interface of the growing bubble was measured by using a time-resolved Particle Tracking Velocimetry (PTV) technique. The results indicate a clear correlation between the magnitude of the Marangoni convection and the electric current.

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Permalink: https://www.hzdr.de/publications/Publ-27230
Publ.-Id: 27230


Noncovalently Assembled Electroconductive Hydrogel

Xu, Y.; Yang, X.ORC; Thomas, A. K.; Patsis, P. A.; Kurth, T.; Kräter, M.; Eckert, K.ORC; Bornhäuser, M.; Zhang, Y.
Crosslinking biomolecules with electroconductive nanostructures through noncovalent interaction can result in modular networks with defined biological functions and physical properties such as electric conductivity and viscoelasticity. Moreover, the resulting matrices can exhibit interesting features caused by the dynamic assembly process, such as self-healing and molecular ordering. In this paper, we present a physical hydrogel system formed by mixing peptide-polyethylene glycol and poly (3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS). This combinatorial approach, which uses different modular building blocks, could lead to high tunability on aspects of rheology and electrical impedance. The proposed physical hydrogel system is characterized by both a self-healing ability and injectability. Interestingly, the formation of hydrogels at relatively low concentrations led to a network of closer molecular packing of PEDOT nanoparticles, reflected by the enhanced conductivity. The biopolymer system can be used to develop 3D cell cultures with incorporated electric stimuli, as evidenced by its contribution to the survival and proliferation of encapsulated mesenchymal stromal cells and their differentiation upon electrical stimulation.
Keywords: self-assembling, PEDOT:PSS, peptide, electroconductive hydrogel, 3D cell

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Permalink: https://www.hzdr.de/publications/Publ-27229
Publ.-Id: 27229


Results of the stationary measurements at COSMEA-I facility - CT part

Bieberle, A.ORC; Boden, S.; Beyer, M.; Hampel, U.

At the COSMEA-I facility cross-sectional distributions of the condensated steam is measured at five different positions along a slightly inclined condensator-tube using adapted conventional CT imaging technique based on X-ray. This data set contains the reconstructed raw data of the CT imaging scans.

Keywords: Passive heat transfer; Conventional CT imaging; Reconstructed raw data of the CT imaging scan
Related publications
Flow morphology and heat transfer analysis during … (Id 29452) is supplemented by this publication
  • Reseach data in the HZDR data repository RODARE
    Publication date: 2018-03-20
    DOI: 10.14278/rodare.3

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Permalink: https://www.hzdr.de/publications/Publ-27228
Publ.-Id: 27228


Molekulare Bildgebung in der Onkologie mittels Positronen-Emissions-Tomographie

Derlin, T.; Grünwald, V.; Steinbach, J.; Wester, H.-J.; Ross, T. L.
Hintergrund: Mit der Positronenemissionstomographie (PET) steht ein Verfahren in der klinischen Bildgebung zur Verfügung, dass bei Durchführung als Hybridverfahren mit Computertomographie (CT) oder Magnetresonanztomographie (MRT) die simultane Erfassung anatomischer und molekularer Informationen ermöglicht. Die PET besitzt eine hohe Sensitivität zur Detektion von Tumormanifestationen. Unterschiedliche Radiopharmaka dienen der Charakterisierung verschiedener Stoffwechselprozesse oder der Analyse der Expression von Rezeptoren, Enzymen und weiteren molekularen Zielstrukturen.
Methode: Selektive Literaturrecherche in PubMed unter Bezug auf nationale und internationale Leitlinien sowie systematische Übersichtsarbeiten und Metaanalysen.
Ergebnisse: Etablierte PET Radiopharmaka wie 2-[18F]Fluor-2-desoxyglukose ([18F]FDG) erlauben die Darstellung physiologischer Prozesse auf molekularer Ebene und können entscheidende Informationen für die klinische Versorgung liefern. Für die PET stehen in zunehmendem Umfang neben gut erforschten und evaluierten auch neuere Radiopharmaka zur nicht-invasiven Phänotypisierung von Tumorerkrankungen zur Verfügung, beispielsweise zur Analyse der Expression des prostataspezifischen Membranantigens (PSMA) oder von Chemokinrezeptoren (z.B. CXCR4) auf Tumorzellen.
Schlussfolgerung: Die PET stellt einen wichtigen Bestandteil diagnostischer Algorithmen in der Onkologie dar, kann die Präzision der Diagnostik verbessern und helfen, die Therapie zu individualisieren. Eine zunehmende Anzahl an PET Radiopharmaka erweitert die verfügbaren Bildgebungsoptionen. Viele Radiopharmaka erlauben neben der nicht-invasiven Analyse der Expression therapeutisch relevanter
Zielstrukturen auch eine nachfolgende zielgerichtete Radionuklidtherapie.

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Permalink: https://www.hzdr.de/publications/Publ-27227
Publ.-Id: 27227


Experimental Signals for Broxen Axial Symmetry in Excited Heavy Nuclei From The Valley of Stability

Grosse, E.; Junghans, A. R.
An increasing number of experimental data indicates the breaking of axial symmetry in many heavy nuclei already in the valley of stability:
Multiple Coulomb excitation analysed in a rotation invariant way, gamma transition rates and energies in odd nuclei, mass predictions, the splitting of Giant Resonances (GR), the collective enhancement of nuclear level densities and Maxwellian averaged neutron capture cross sections. For the interpretation of these experimental observations, the axial symmetry breaking shows up in nearly all heavy nuclei as predicted by Hartree–Fock–Bogoliubov (HFB) calculations; this indicates a nuclear Jahn–Teller effect.
We show that nearly no parameters remain free to be adjusted by separate fitting to level density or giant resonance data, if advance information on nuclear deformations, radii etc. are taken from such calculations with the force parameters already fixed. The data analysis and interpretation have to include the quantum mechanical requirement of zero point oscillations and the distinction between static vs. dynamic symmetry breaking has to be regarded.
  • Open Access Logo Contribution to proceedings
    XXIV Nuclear Physics Workshop “Marie and Pierre Curie”, Kazimierz Dolny, Poland, September 20–24, 2017., 20.-24.09.2017, Kazimierz Dolny, Polen
    Acta Physica Polonica B, Vol. 11, No. 1-37
    DOI: 10.5506/APhysPolBSupp.11.37

Permalink: https://www.hzdr.de/publications/Publ-27226
Publ.-Id: 27226


Diffusion of oxygen in bcc Fe under the influence of other foreign atoms

Wang, X.; Posselt, M.; Faßbender, J.
First-principle calculations and kinetic Monte Carlo simulations are applied to investigate the diffusion of oxygen in bcc Fe under the influence of other foreign atoms, such as Al, Si, P, S, Ti,, Cr, Mn, Ni, Y, and Mo. In the first part of this work jumps of oxygen in pure bcc Fe, between first-, second-, and third-neighbor octahedral interstitial sites were investigated by DFT. It is found that a second-neighbor jump consists of two consecutive first-neighbor jumps and that the barrier of the third-neighbor jump is too high to be relevant. In the second part DFT was applied to determine the modified migration barriers, i.e. for the oxygen jump between the first and the second neighbor of a foreign atom, etc. It is found that Si, P, Ni and Mo influence the migration barriers of oxygen only slightly. Al and Cr cause moderate changes, while S, Ti, and Y lead to strong modifications. With the exception of Y the migration paths are first-neighbor jumps between (modified) octahedral sites with (modified) tetrahedral sites as saddle points. Y changes some migration paths considerably. Using the migration barriers calculated by DFT the diffusion coefficient of oxygen was determined by kinetic Monte Carlo simulations considering a dilute iron alloy. In general the foreign atoms cause a reduction of the mobility of oxygen compared to that in pure bcc Fe. The strongest decrease is obtained for the foreign atoms S, Ti, and Y.
Keywords: Diffusion, oxygen, bcc Fe, Density Functional Theory, Kinetic Monte Carlo simulations
  • Poster
    DPG-Frühjahrstagung und EPS-CMD27, 11.-16.03.2018, Berlin, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-27225
Publ.-Id: 27225


Structure and energetics of Y-Ti-O nanoclusters in bcc Fe

Vallinayagam, M.; Posselt, M.; Faßbender, J.
In this research project the nature of yttria-based oxide nanoclusters in a bcc Fe matrix is investigated by DFT calculations. The main goal of these studies is the better understanding of the nucleation as well as the structure and composition of the clusters.
In the first part of the work three types of structures are considered: (i) clusters consisting of parts of the bixbyite (Y2O3) or pyrochlore (Y2Ti2O7) structure embedded in bcc Fe, (ii) clusters with Y, Ti, and O on substitutional sites, and (iii) clusters with of Y, Ti, on substitutional sites and O on octahedral interstitial sites of the bcc lattice. Simulation cells containing different structures but the same composition of atoms (Fe, Y, Ti, O) are compared. It is found that the energetics of three different structure types, i.e. their total binding energy, is very similar. This modifies the statement of Barnard et al. [1] who only considered the first type of structure and concluded that this is the most favorable. Further, more stable cluster structures are constructed using another model with the nanocluster core similar to the metal monoxide structure. Also the binding energy of monomers like O, Y, Ti, and the vacancy to the cluster are studied. O and the vacancy are strongly attracted by the nanoclusters, while the interaction with metal atoms is weaker.
[1] L. Barnard et al. Acta Mater. 60 935 (2012)
Keywords: Density Functional Theory, Y-Ti-O nanoclusters, bcc Fe
  • Poster
    DPG-Frühjahrstagung und EPS-CMD27, 11.-16.03.2018, Berlin, Deustchland

Permalink: https://www.hzdr.de/publications/Publ-27224
Publ.-Id: 27224


The role of radiative de-excitation in the neutralization process of highly charged ions interacting with a single layer of graphene

Schwestka, J.; Wilhelm, R. A.ORC; Gruber, E.; Heller, R.; Kozubek, R.; Schleberger, M.; Facsko, S.; Aumayr, F.
X-ray emission of slow (<1 a.u.) highly charged Argon and Xenon ions is measured for transmission through a freestanding single layer of graphene. To discriminate against X-ray emission originating from the graphene's support grid a coincidence technique is used. X-ray emission of 75 keV Ar17+ and Ar18+ ions with either one or two K-shell vacancies is recorded. Using a windowless Bruker XFlash detector allows us to measure additionally Ar KLL and KLM Auger electrons and determine the branching ratio of radiative vs. non-radiative decay of Ar K-shell holes. Furthermore, X-ray spectra for 100 keV Xe22+-Xe35+ ions are compared, showing a broad M-line peak for all cases, where M-shell vacancies are present. All these peaks are accompanied by emission lines at still higher energies indicating the presence of a hollow atom during X-ray decay. We report a linear shift of the main M-line peak to higher energies for increasing incident charge state, i.e. increasing number of M-shell holes.
Keywords: Slow highly charged ions; Graphene; X-ray emission

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Permalink: https://www.hzdr.de/publications/Publ-27223
Publ.-Id: 27223


Structural incorporation of the minor actinide Cm(III) in La1-xGdxPO4 rhabdophane and monazite solid solutions

Huittinen, N.; Scheinost, A. C.; Ji, Y.; Kowalski, P. M.; Arinicheva, Y.; Wilden, A.; Neumeier, S.
Monazites (LnPO4) are envisioned as potential immobilization matrices for high-level radioactive wastes produced e.g. during the nuclear fuel cycle [1–2]. Hydrated rhabdophane (LnPO4×0.67H2O) is a precursor phase during monazite synthesis and a potential solubility-limiting solid phase under nuclear waste storage conditions [3–4]. Thus, for a reliable long-term safety assessment of nuclear waste repositories for conditioned radioactive waste, a fundamental understanding of the radionuclide incorporation process in both the pristine monazite ceramics and their alteration products is required.

In the present study we have combined time-resolved laser fluorescence spectroscopy (TRLFS), X-ray Absorption Fine Structure (XAFS) spectroscopy and ab initio atomistic simulations to investigate the structural incorporation of the minor actinide curium in synthetic La1-xGdxPO4 monazite and rhabdophane solid solutions. The solid phase was synthesized by addition of phosphoric acid to a solution containing La3+ and Gd3+ in desired relative concentrations and a small amount of the actinide (248Cm), until a white precipitate of La1-xGdxPO4 rhabdophane doped with approximately 50 ppm Cm3+ was obtained. An aliquot of the obtained solid phase was thereafter sintered at 1450°C to acquire the crystalline monazite ceramic. Structural refinement of collected XRD data for both rhabdophane and monazite solids show a linear dependency of lattice parameters as a function of Gd3+ substitution according to Vegard’s law.
Our combined spectroscopic results show that Cm3+ is incorporated in the monazite end-members (LaPO4 and GdPO4) on one specific, highly ordered lattice site. In the intermediate solid solution compositions, an increasing disorder around the Cm3+ dopant can be seen as a result of a broader distribution of possible Cm∙∙∙O bond-lengths in comparison to the end-member compositions with very well-defined nearest neighbour distances. Despite this local structural disordering, homogenous solid solutions were obtained for all synthesized monazite compositions without the formation of dopant clusters that could potentially hamper the performance of the monazite ceramics for the immobilization of minor actinide containing wastes.
The hydrated rhabdophane lattice comprises two different site types that could accommodate the actinide dopant: a 9-coordinated “hydrated” site amounting to two thirds (2/3) of the total number of lanthanide sites in the solid structure, where one coordinating oxygen atom originates from a water molecule, and an 8-fold coordinated “non-hydrated” site (1/3 of available Ln sites) where all oxygen atoms are provided by phosphate groups [4]. Based on our laser spectroscopic investigation, curium incorporation on both site types can be confirmed, however, the site occupancy is not in concordance with the hydrated rhabdophane structure. In contrast, a preferential incorporation of curium on non-hydrated lattice sites can be seen, especially for the La-rich rhabdophane compositions, implying that structural substitution reactions cannot be predicted based on the structure of the host matrix only.
Keywords: Cm(III), spectroscopy, incorporation, rhadbophane, monazite
  • Lecture (Conference)
    International Symposium on Solubility Phenomena and Related Equilibrium Processes (ISSP), 15.-20.07.2018, Tours, France

Permalink: https://www.hzdr.de/publications/Publ-27222
Publ.-Id: 27222


Unusual Coulomb effects in graphene

Winnerl, S.
In many semiconductors Coulomb scattering plays an essential role in the thermalization process of a non-equilibrium carrier distribution. Here we discuss three surprising and fascinating manifestations of Coulomb scattering in graphene. All phenomena are explored both experimentally and by manybody theory. The first observation concerns a double-bended saturation behavior of bleaching induced by near-infrared radiation. The second phenomenon is the optically induced anisotropy in k-space for excitation with linearly polarized radiation and its relaxation to a Fermi-Dirac distribution. The third set of experiments tackles the dynamics of graphene in a magnetic field perpendicular to the graphene layer. Here evidence for strong Auger scattering is found. We discuss the possibility to apply Landau quantized graphene as a gain medium in a tunable laser and as a tunable nonlinear optical material.
Keywords: Graphene, ultrafast dynamics, Coulomb interaction
  • Lecture (others)
    Theory seminar, Charles University in Prague, 12.04.2018, Prague, Czech Repzblic

Permalink: https://www.hzdr.de/publications/Publ-27221
Publ.-Id: 27221


Intrinsic magnetic properties of hydrided and non-hydrided Nd5Fe17 single crystals

Karpenkov, D. Y.; Skokov, K. P.; Lyakhova, M. B.; Radulov, I. A.; Faske, T.; Skourski, Y.; Gutfleisch, O.
We report on the spontaneous magnetization Ms, the exchange stiffness constant A and the magneto-crystalline anisotropy constants K1, K2, K3 and K4 of Nd5Fe17 and Nd5Fe17H16 single crystals. Field dependencies of magnetization M(H) were measured along a, b' and c principal crystallographic directions within the temperature range of 10-600 K and magnetic fields up to 40 T. Large anisotropies of spontaneous magnetization and high-field susceptibility were revealed for both compounds. The exchange stiffness parameter A was determined using Bloch's T3/2 law. In order to provide high accuracy detection of K1(T), K2(T), K3(T) and K4(T), we used two different approaches: the modified Sucksmith-Thompson technique and the Néel's phase method.

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Permalink: https://www.hzdr.de/publications/Publ-27220
Publ.-Id: 27220


Electrically pumped graphene-based Landau-level laser

Brem, S.; Wendler, F.; Winnerl, S.; Malic, E.
Graphene exhibits a nonequidistant Landau quantization with tunable Landau-level (LL) transitions in the technologically desired terahertz spectral range. Here, we present a strategy for an electrically driven terahertz laser based on Landau-quantized graphene as the gain medium. Performing microscopic modeling of the coupled electron, phonon, and photon dynamics in such a laser, we reveal that an inter-LL population inversion can be achieved resulting in the emission of coherent terahertz radiation. The presented paper provides a concrete recipe for the experimental realization of tunable graphene-based terahertz laser systems.
Keywords: graphene, Landau quantization, laser, Landau-level laser

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Permalink: https://www.hzdr.de/publications/Publ-27219
Publ.-Id: 27219


ThMn12-type phases for magnets with low rare-earth content: Crystal-field analysis of the full magnetization process

Tereshina, I. S.; Kostyuchenko, N. V.; Tereshina-Chitrova, E. A.; Skourski, Y.; Doerr, M.; Pelevin, I. A.; Zvezdin, A. K.; Paukov, M.; Havela, L.; Drulis, H.
Rare-earth (R)-iron alloys are a backbone of permanent magnets. Recent increase in price of rare earths has pushed the industry to seek ways to reduce the R-content in the hard magnetic materials. For this reason strong magnets with the ThMn12 type of structure came into focus. Functional properties of R(Fe,T)12 (T-element stabilizes the structure) compounds or their interstitially modified derivatives, R(Fe,T)12-X (X is an atom of hydrogen or nitrogen) are determined by the crystal-electric-field (CEF) and exchange interaction (EI) parameters. We have calculated the parameters using high-field magnetization data. We choose the ferrimagnetic Tm-containing compounds, which are most sensitive to magnetic field and demonstrate that TmFe11Ti-H reaches the ferromagnetic state in the magnetic field of 52 T. Knowledge of exact CEF and EI parameters and their variation in the compounds modified by the interstitial atoms is a cornerstone of the quest for hard magnetic materials with low rare-earth content.

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Publ.-Id: 27218


Field-effect transistors as electrically controllable nonlinear rectifiers for the characterization of terahertz pulses

Lisauskas, A.; Ikamas, K.; Massabeau, S.; Bauer, M.; Cibiraité, D.; Matukas, J.; Mangeney, J.; Mittendorff, M.; Winnerl, S.; Krozer, V.; Roskos, H. G.
We propose to exploit rectification in field-effect transistors as an electrically controllable higher-order nonlinear phenomenon for the convenient monitoring of the temporal characteristics of THz pulses, for example, by autocorrelation measurements. This option arises because of the existence of a gate-bias-controlled super-linear response at sub-threshold operation conditions when the devices are subjected to THz radiation. We present measurements for different antenna-coupled transistor-based THz detectors (TeraFETs) employing (i) AlGaN/GaN high-electron-mobility and (ii) silicon CMOS field-effect transistors and show that the super-linear behavior in the sub-threshold bias regime is a universal phenomenon to be expected if the amplitude of the high-frequency voltage oscillations exceeds the thermal voltage. The effect is also employed as a tool for the direct determination of the speed of the intrinsic TeraFET response which allows us to avoid limitations set by the read-out circuitry. In particular, we show that the build-up time of the intrinsic rectification signal of a patch-antenna-coupled CMOS detector changes from 20 ps in the deep sub-threshold voltage regime to below12 ps in the vicinity of the threshold voltage.
Keywords: Terahertz detection, field-effect transistor, nonlinear response, autocorrelation

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Publ.-Id: 27217


Infrared/Terahertz Spectra of the Photogalvanic Effect in (Bi,Sb)Te based Three Dimensional Topological Insulators

Plank, H.; Pernul, J.; Gebert, S.; Danilov, S. N.; König-Otto, J.; Winnerl, S.; Lanius, M.; Kampmeier, J.; Mussler, G.; Aguilera, I.; Grützmacher, D.; Ganichev, S. D.
We report on the systematic study of infrared/terahertz spectra of photocurrents in (Bi,Sb)Te based three dimensional topological insulators. We demonstrate that in a wide range of frequencies, ranging from fractions up to tens of terahertz, the photocurrent is caused by the linear photogalvanic effect (LPGE) excited in the surface states. The photocurrent spectra reveal that at low frequencies the LPGE emerges due to free carrier Drude-like absorption. The spectra allow to determine the room temperature carrier mobilities in the surface states despite the presence of thermally activated residual impurities in the material bulk. In a number of samples we observed an enhancement of the linear photogalvanic effect at frequencies between 30 and 60 THz, which is attributed to the excitation of electrons from helical surface to bulk conduction band states. Under this condition and applying oblique incidence we also observed the circular photogalvanic effect driven by the radiation helicity.
Keywords: Topological insulators, terahertz spectroscopy, photocurrents, photogalvanic effect

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Permalink: https://www.hzdr.de/publications/Publ-27216
Publ.-Id: 27216


Shielding and source calculations for the new cyclotron and possible activation in the soil

Konheiser, J.; Ferrari, A.; Naumann, B.; Müller, S.
This presentation summarizes the results of the Monte Carlo simulation of the shielding calculations and estimates of the soil activation for the new cyclotron of the HZDR (Helmholtz-Zentrum Dresden-Rossendorf). The dose values were determined on base of the resulting neutron flux at the 18F production and were carried out with the Monte Carlo code MCNP6. The calculation of the soil activations was performed with FLUKA. The neutron source term was provided by manufacturer. A source check with MCNP6 and FLUKA codes, significant discrepancies were found to the manufacturer supplied data for the neutron source term. For this reason, experiments were carried out on a cyclotron in operation. The comparison confirmed the results of the MCNP/FLUKA calculations.
The estimated dose rate in the public area is about 0.035 μSv/h (28 MeV protons) and thus significantly below the reference value of 0.5 μSv/h(3). After 5 years of continuous beam operation and a subsequent decay time of 30 days, the activity concentration of the soil is about 0.34 Bq/g.
Keywords: shielding calculation, neutron source calculation, cyclotron, MCNP6, FLUKA
  • Lecture (others)
    88. Sitzung des Arbeitskreises Dosimetrie, 20.-21.03.2018, TU Dresden, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-27215
Publ.-Id: 27215


Transglutaminase 2 as potential target for functional tumour imaging – development of assay methods and inhibitors for this enzyme

Wodtke, R.
Transglutaminase 2 (TGase 2) is a unique multifunctional enzyme whose best-characterised function is the crosslinking of proteins, which has implications not only in physiological but also in a variety of pathological conditions including fibrotic and neoplastic processes. In this context, it becomes more and more apparent that TGase 2 is a key player for the progression of several kinds of cancer and elevated levels of TGase 2 expression are directly correlated with poor prognostic indicators for survival, e.g. metastatic phenotype and drug resistance of the cancer cells. Consequently, this enzyme is considered as a promising target for the diagnosis and therapy of these diseases. According to the motivation to develop radiotracers for TGase 2 imaging by positron emission tomography (PET), which will provide insight into the importance of the crosslinking function as well as the targeting of that enzyme in vivo, the PhD project was focused on two different goals.
Within the first part, a reliable fluorimetric assay method was established as prerequisite for the identification and characterisation of TGase 2-reactive molecules. The assay is based on the measurement of an increase in fluorescence due to the release of a coumarine derivative upon TGase 2-catalysed hydrolysis or aminolysis of the fluorogenic acyl donor. However, the fluorogenic acyl donors known from the literature are characterised by a low solubility in water, which limits their applicability (1). Therefore, a series of water-soluble small peptidic acyl donors were synthesised and kinetically characterised towards TGase 2. Finally, Z-Glu(HMC)-Gly-OH turned out to have the most favourable substrate properties (2). Additionally, this compound is also a suitable substrate for other TGases, which facilitates selectivity studies.
The second part was focused on irreversible inhibitors for TGase 2 as appropriate starting point for the development of radiotracers. Based on the Nε-acryloyllysine piperazides chemotype of TGase 2 inhibitors, a library of >50 inhibitors were synthesised and their inhibitory capacity towards TGase 2 and other TGases were determined on the basis of their inactivation constants kinact/KI. Structural modifications were focused on the introduction of fluorine but also other chemical groups were considered. Kinetic investigations have uncovered important structure-activity relationships, which in combination with in silico molecular docking shed light on the binding mode for this class of inhibitors. Evaluation of selected compounds at other TGases highlighted a favourable selectivity profile towards TGase 2. Regarding an initial pharmacokinetic profiling, the potential membrane permeability of the inhibitors were determined using the PAMPA method. Considering the determined inhibitory potencies in combination with these pharmacokinetic in vitro data will provide valuable hints for the development of radiotracers for TGase 2 imaging.

(1) Gillet, S. M.; Pelletier, J. N.; Keillor, J. W. Anal. Biochem. 2005, 347, 221.
(2) Wodtke et al. ChemBioChem 2016, 17, 1263.
  • Invited lecture (Conferences)
    Frontiers in Medicinal Chemistry, Verleihung Promotionspreis der GDCh-Fachgruppe Medizinische Chemie, 11.-14.03.2018, Jena, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-27213
Publ.-Id: 27213


Anwendung von Anstaupackungen bei der CO2-Absorption in wässrigen Aminlösungen

Flechsig, S.; Sohr, J.; Schubert, M.; Hampel, U.; Kenig, E. Y.
Kolonneneinbauten stellen einen wichtigen Bestandteil fluider Trennprozesse dar und haben einen erheblichen Einfluss auf die Prozessleistung. Anzustrebende Eigenschaften von Einbauten sind eine hohe Trenneffizienz bei gleichzeitig geringem Druckverlust sowie eine hohe Kapazität. In den vergangenen Jahrzehnten konnten erhebliche Fortschritte zur Verbesserung von Einbauten erzielt werden. In diesem Bereich zeigt die Entwicklung von Anstaupackungen (AP) ein wesentliches Potenzial zur Prozessintensivierung auf. Diese bestehen aus zwei alternierenden Lagen strukturierter Packungen mit unterschiedlicher spezifischer Oberfläche. Die untere Anstaulage weist eine geringere Lastgrenze als die darüber angeordnete Abscheidelage auf. AP werden üblicherweise zwischen den Flutpunkten der beiden Lagen betrieben, weshalb ein heterogenes Strömungsmuster entsteht. Dabei bildet sich oberhalb der gefluteten Anstaulage eine Sprudelschicht, die durch eine intensive Vermischung der Phasen geprägt ist und eine hohe Trennleistung erzielt.
Im Rahmen eines DFG-geförderten Forschungsprojekts gilt es nun, die Auswirkungen der einzelnen Strömungsregime von AP auf Fluiddynamik und Stofftransport separat zu untersuchen. Für diesen Zweck werden erstmalig Experimente an einer Absorptions-/ Desorptionsanlage durch bildgebende Messungen der Strömung in AP ergänzt. An der Universität Paderborn werden für verschiedene Design- und Betriebsparameter Technikumsversuche zur CO2-Absorption in einer wässrigen Monethanolamin-Lösung durchgeführt. Die Anlage ermöglicht die Aufnahme von Temperaturprofilen der Gasphase sowie von Konzentrationsprofilen beider Phasen. In Kooperation mit der Technischen Universität Dresden wird mittels ultraschneller Röntgentomographie ein detaillierter Einblick in die Phasenverteilung der verschiedenen Strömungszustände ermöglicht. Die bei beiden Untersuchungen anfallenden Messdaten sollen zur Erarbeitung von Korrelationen für Stoffübergang, Phasengrenzfläche, Holdup und Druckverlust genutzt werden, welche in einem rate-based-Model Verwendung finden. In dieser Arbeit werden neben einer Vorstellung des Vorhabens erste experimentelle Daten zur Absorption mit AP präsentiert.
  • Poster
    Jahrestreffen der ProcessNet Fachgruppen Mechanische Flüssigkeitsabtrennung, Kristallisation, Phytoextrakte, Adsorption, Extraktion, Fluidverfahrenstechnik und Membrantechnik, 08.-10.03.2017, Köln, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-27212
Publ.-Id: 27212


Experimentelle Untersuchungen zum Einfluss von Betriebs- und Designparameter auf das Absorptionsverhalten von Anstaupackungen

Flechsig, S.; Utchenko, Y.; Sohr, J.; Schubert, M.; Hampel, U.; Kenig, E. Y.
Aufgrund des hohen Energiebedarfs thermischer Trennverfahren besteht ein hoher Forschungsbedarf für die Entwicklung effizienter und ressourcenschonender Prozesse. Bei Trennkolonnen weisen Einbauten ein erhebliches Entwicklungspotential auf, welche die Fluiddynamik und den Stofftransport entscheidend beeinflussen.
Die Anstaupackung stellt eine Entwicklung im Bereich der Packungskolonnen dar, die eine Intensivierung des Stofftransports und eine Kapazitätserweiterung ermöglicht. Die Anstaupackung besteht aus einer Kombination von zwei Lagen typischer strukturierter Packungen mit unterschiedlicher spezifischer Oberfläche, welche alternierend angeordnet werden. Die untere Anstaulage weist dabei eine geringere Lastgrenze als die darüber angeordnete Abscheidelage auf. Anstaupackungen werden üblicherweise zwischen den Flutpunkten der beiden Lagen betrieben, wodurch ein axial heterogenes Strömungsmuster entsteht. Dabei bildet sich oberhalb der gezielt gefluteten Anstaulage eine Sprudelschicht, die durch eine intensive Vermischung und ein hohes Maß an Turbulenz der beteiligten Phasen geprägt ist und zu deutlich höheren Trennleistungen führen kann. Oberhalb der Sprudelschicht in der Abscheidelage dominiert die für Packungen typische Rieselfilmströmung in der die aus der Sprudelschicht mitgerissenen Tropfen abgeschieden werden [1].
Da bislang das Trennverhalten von Anstaupackung fast ausschließlich theoretisch analysiert wurde [2], werden im Rahmen eines von der DFG geförderten Kooperationsprojekts die Auswirkungen der einzelnen Strömungsregime auf Fluiddynamik und Stofftransport komplementär sowohl experimentell als auch theoretisch untersucht. Für diesen Zweck werden erstmalig Experimente an einer Absorptions-/ Desorptionsanlage durch bildgebende Messungen der Strömung in Anstaupackungen ergänzt. An der Universität Paderborn werden für verschiedene Design- und Betriebsparameter Technikumsversuche zur CO2-Absorption in einer wässrigen Monoethanolamin-Lösung durchgeführt. Die Anlage ermöglicht die Aufnahme von Temperaturprofilen der Gasphase sowie von Konzentrationsprofilen beider Phasen. Am Helmholtz-Zentrum Dresden-Rossendorf wird mittels ultraschneller Röntgentomographie ein detaillierter Einblick in die Phasenverteilung der verschiedenen Strömungszustände ermöglicht. Die Messdaten beider Projektpartner werden zur Erarbeitung von Korrelationen für Stoffübergang, Phasengrenzfläche, Holdup und Druckverlust genutzt, welche in einem rate-based-Model Verwendung finden.
Im Rahmen dieser Arbeit wird der Einfluss wichtiger Betriebs- und Designparameter auf das Absorptionsverhalten in Anstaupackungen experimentell untersucht, um einerseits effizienzsteigernde Betriebsbedingungen zu identifizieren und anderseits eine Basis für die experimentelle Validierung von neuen Simulationsmodellen zu schaffen. Zusätzlich wird eine empirische Korrelationsgleichung zur Bestimmung des integralen Stoffdurchgangskoeffizienten entwickelt, die den Einfluss der Temperatur des Lösungsmittels, der Gas- und Flüssigkeitsbelastung, der CO2-Konzentration im Rohgas sowie der MEA-Konzentration in der Lösung berücksichtigt. Die vorgeschlagene Korrelation ermöglicht damit eine überschlägige Auslegung von Absorptionskolonnen mit Anstaupackungen.

[1] U. Brinkmann, B. Kaibel, M. Jödecke, J. Mackowiak, E.Y. Kenig: Beschreibung der Fluiddynamik von Anstaupackungen, Chemie Ingenieur Technik 84: 36-45 (2012).
[2] Ö. Yildirim, E.Y. Kenig: Rate-based modelling and simulation of distillation columns with sandwich packings, Chemical Engineering and Processing: Process Intensification 98, 147-154 (2015).
  • Lecture (Conference)
    Jahrestreffen der Fachgemeinschaft Prozess-, Apparate- und Anlagentechnik, 20.-21.11.2017, Würzburg, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-27211
Publ.-Id: 27211


Rate-based-Modellierung von CO2-Absorptionskolonnen mit Anstaupackungen

Flechsig, S.; Sohr, J.; Schubert, M.; Hampel, U.; Kenig, E. Y.
Eines der am häufigsten eingesetzten Trennverfahren zur Abscheidung von Kohlenstoffdioxid (CO2) aus Kraftwerksabgasen ist die Reaktivabsorption mit wässrigen Aminlösungen. Neben der Entwicklung effektiverer Lösungsmittel weisen die Kolonneneinbauten hinsichtlich Druckverlust, Kapazität und Trennleistung ein wesentliches Potenzial für die Prozessintensivierung und damit die Reduzierung des hohen Ressourcenbedarfs auf.
Eine Verbesserung der Trennleistung kann durch den Einsatz von Anstaupackungen erzielt werden. Diese bestehen aus zwei abwechselnden Lagen von Standardpackungen mit unterschiedlichen spezifischen Oberflächen. Die untere Packungslage (die sogenannte Anstaulage) hat eine geringere Belastungsgrenze im Vergleich zur darüberliegenden Abscheidelage. Anstaupackungen werden typischerweise bei Betriebsbedingungen zwischen den Flutpunkten beider Lagen betrieben. Durch das gezielte Fluten der Anstaulage bildet sich eine in die Abscheidelage hineinreichende Sprudelschicht, in der eine hohe Trennleistung mit intensiver Phasenvermischung erzielt wird. Im oberen Bereich der Abscheidelage können filmähnliche Strömungsmuster, Rinnsale und aus der Sprudelschicht mitgerissene Tropfen beobachtet werden [1]. Obwohl der für Trennverfahren vorteilhafte intensive Phasenkontakts bei dem integrierten Packungstyps bereits nachgewiesen wurde, fehlend validierte Auslegungsgrundlagen für eine breitere Anwendung [2].
Eine genaue Vorhersage der Leistungscharakteristik ist für die Auslegung von Anstaupackungen unerlässlich. In einem von der DFG geförderten Kooperationsprojekt zwischen Universität Paderborn und TU Dresden werden die Auswirkungen der einzelnen Strömungsregime auf die Fluiddynamik und den Stoffaustausch komplementär mit experimentellen und theoretischen Methoden untersucht. Um die Auswirkungen jedes einzelnen Strömungsregimes zu bestimmen, werden Experimente an einer Absorptions-/ Desorptionsanlage durch bildgebende Messungen in Anstaupackungen ergänzt. An der Universität Paderborn wird die CO2-Absorption in einer Pilotanlage für verschiedene Design- und Betriebsparameter untersucht. Die Anlage ermöglicht die Messung von Temperaturprofilen der Gasphase sowie von Konzentrationsprofilen beider Phasen. Mithilfe der ultraschnellen Röntgentomographie wird am Helmholtz-Zentrum Dresden-Rosendorf die Phasenverteilung innerhalb der Anstaupackung untersucht. Die Messdaten aus beiden experimentellen Methoden werden verwendet, um Korrelationen für Stofftransportkoeffizienten, Phasengrenzfläche, Holdup und Druckverlust zu entwickeln, die in einem rate-based-Modell für CO2-Absorptionsverfahren mit wässrigen Aminlösungen eingesetzt werden.
Der rate-based-Ansatz kann die Besonderheiten diverser Kolonneneinbauten durch einbautenspezifische Korrelationen berücksichtigen. Da die verschiedenen Fluiddynamikregime in Anstaupackungen unterschiedliche Auswirkungen auf den Stofftransport aufweisen, werden Absorptionskolonnen mit Anstaupackungen als eine Folge von abwechselnden Segmenten dargestellt und jedes Segment wird durch einen der Fluiddynamik entsprechenden Satz von Korrelationen beschrieben. Im Rahmen dieser Arbeit erfolgt eine Validierung des Modells mit experimentellen Daten zur CO2-Absorption.

[1] U. Brinkmann, B. Kaibel, M. Jödecke, J. Mackowiak, E.Y. Kenig: Beschreibung der Fluiddynamik von Anstaupackungen, Chemie Ingenieur Technik 84: 36-45 (2012).
[2] Ö. Yildirim, E.Y. Kenig: Rate-based modelling and simulation of distillation columns with sandwich packings, Chemical Engineering and Processing: Process Intensification 98, 147-154 (2015).
  • Lecture (Conference)
    Jahrestreffen der ProcessNet-Fachgruppe Fluidverfahrentechnik, 27.-28.02.2018, München, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-27210
Publ.-Id: 27210


New Phenomena in Gamma-Ray Strength Functions

Schwengner, R.
The excitation and deexcitation of atomic nuclei by electromagnetic radiation are fundamental processes in reactions of this many-body quantum system. At high excitation energy and high level density, statistical models are applied to describe reaction rates, which use $\gamma$-ray strength functions (γSF) to describe the average transition probabilities in a certain range of excitation energy. The experimental determination and the theoretical understanding of the properties of γSF are important for the accurate description of photonuclear reactions and radiative-capture reactions, which play a central role in the synthesis of the elements in various stellar environments.
We report photon-scattering experiments using bremsstrahlung at the γELBE facility (HZDR) and quasi-monoenergetic, polarized γ beams at the HIγS facility (TUNL, Duke Univ., Durham, USA). Systematic studies of the dipole strength revealed new phenomena that are not described by the analytical approximations currently used in reaction codes. The (γ,γ') experiments at high energy show considerable contributions to the γSF from the quasicontinuum of states. Combined with (γ,n) cross sections, the (γ,γ') data provide experimental input γSF for statistical reaction codes.
Keywords: Photonuclear reactions, Nuclear resonance fluorescence, Bremsstrahlung, Monoenergetic gamma rays, Shell Model.
  • Invited lecture (Conferences)
    Frühjahrstagung 2018, 26.02.-02.03.2018, Bochum, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-27208
Publ.-Id: 27208


Damage accumulation and structural modification in c-plane and a-plane GaN implanted with 400 keV Kr and Gd ions

Mackova, A.; Malinsky, P.; Jágerova, A.; Sofer, Z.; Klímová, K.; Sedmidubský, D.; Mikulics, M.; Böttger, R.; Akhmadaliev, S.
GaN is the most actively studied wide-bandgap material, applicable e.g. in short-wavelength optoelectronic devices, high-electron-mobility transistors, and semiconductor lasers. The crystallographic orientation of an implanted crystal can significantly influence the optical properties of the implanted layer, reflecting the rearrangement of the crystal matrix after annealing. The annealing procedure, influencing dynamic recovery, point defect diffusion and large defect stabilisation, depending on the GaN crystal orientation and the used ion implantation parameters, is still an important issue to be studied. We have studied the structural and compositional changes of the GaN-epitaxial-layers of c-plane and a-plane orientations grown by MOVPE and implanted with Gd and Kr ions using the ion energy of 400 keV and ion fluences of 5 × 1014 cm-2, 1 × 1015 cm-2 and 5 × 1015 cm-2 with subsequent annealing at 800 °C in ammonia. Dopant depth profiling was accomplished by Rutherford backscattering spectrometry (RBS). Induced structure disorder and its recovery during subsequent annealing were characterised by RBS channelling and Raman spectroscopy. Ion-implanted c-plane and a-plane GaN exhibit significant differences in damage accumulation simultaneously with post-implantation annealing, inducing a different structural reorganization of the GaN structure in the buried layer depending on the introduced disorder level, i.e. depending on the ion-implantation fluence and ion mass.
Keywords: GaN damage accumulation, RBS channelling studies of implanted GaN, Structure modification in c-plane and a-plane GaN

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Permalink: https://www.hzdr.de/publications/Publ-27207
Publ.-Id: 27207


Damage accumulation and structural modification in a- and c-plane GaN implanted with 400-keV and 5-MeV Au+ ions

Mackova, A.; Malinsky, P.; Jágerova, A.; Sofer, Z.; Sedmidubský, D.; Klímová, K.; Böttger, R.; Akhmadaliev, S.
c-plane (0001) and a-plane (11-20) gallium nitride (GaN) epitaxial layers were grown by Metal organic Vapour Phase epitaxy (MOVPE) on sapphire and subsequently implanted with 400-keV and 5-MeV Au+ ions using fluences 5 × 1014 to 5 × 1015 cm-2. The shallow Au depth profiling was accomplished by Rutherford backscattering spectrometry. The structural changes during implantation and subsequent annealing were characterised by Rutherford backscattering spectrometry channelling and Raman spectroscopy. The interplay between nuclear and electronic stopping, influencing defect accumulation, was monitored and discussed depending on GaN orientation. Post-implantation annealing induced a structural reorganisation of the GaN structure depending on the ion-implantation fluence, ion energy, and on the crystallographic orientation.
Keywords: damage accumulation in GaN, RBS channelling in ion-modified GaN, structure modification in c-plane and a-plane GaN

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Permalink: https://www.hzdr.de/publications/Publ-27206
Publ.-Id: 27206


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