Publications Repository - Helmholtz-Zentrum Dresden-Rossendorf

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35836 Publications

Application of computational fluid dynamics codes for nuclear power plant design

Krause, M.; Smith, B.; Höhne, T.; In, W. K.

Computational Fluid Dynamics (CFD) codes have reached a level of maturity, at least for single-phase applications, to be utilized in the design process of Nuclear Power Plant (NPP) components, such that advanced NPPs over the past years have increasingly utilized CFD codes in their design. A recently completed Cooperative Research Project (CRP) addressed the application of CFD codes to the process of optimizing the design of components in Pressurized Water-cooled Reactors (PWRs). Following several initiatives within the IAEA where CFD codes have been applied to situations of interest in nuclear reactor technology, this CRP aimed to contribute to a consistent application of CFD codes by establishing a common platform to assess their capabilities and level of qualification.

Eleven participant organizations from nine Member States performed simulations against four “CFD-grade” experiments performed to investigate key phenomena for CFD simulations. Two are based on test data from the ROCOM (ROssendorf COolant Mixing) facility at HZDR in Germany, and another two are based on rod-bundle experiments in the OFEL (Omni Flow Experimental Loop) facility at KAERI in Korea.

This paper outlines the objectives of the CRP, provides a description of the test facilities and experiments, and discusses selected results obtained for the four above benchmark exercises.

Keywords: Computational Fluid Dynamics; Reactor Design; CFD Benchmark

  • Lecture (Conference)
    18th International Topical Meeting on Nuclear Reactor Thermal Hydraulics (NURETH-18), 18.-23.08.2019, Portland, USA
  • Contribution to proceedings
    18th International Topical Meeting on Nuclear Reactor Thermal Hydraulics (NURETH-18), 18.-23.08.2019, Portland, USA

Publ.-Id: 29046

Perfluorinated Calixarene Shuttles for Radium and Barium

Reissig, F.; Bauer, D.; Pietzsch, H.-J.; Steinbach, J.; Mamat, C.

Alpha therapy is continually discussed in radiopharmaceutical research. [223Ra]RaCl2 is the only EMA- and FDA-approved alpha-emitting radiopharmaceutical so far. Since the use of 223Ra is only based on its calcimimetic behavior. It is directly bond to bone structures in the body. To enhance the therapeutic potential of radium isotopes, it is necessary to develop novel carrier systems for radium ions as a base of biological targeting units. By the combination of 223Ra or 224Ra, which both have suitable physical half-lives for therapeutic applications, and 131Ba which has a similar half-life but diagnostic radiation properties, a theragnostic idea can also be followed. Our project aims at the synthesis of calixarene-based ligands for the stable complexation of barium and radium ions. Recent studies in our group have already shown the high potential of such ligands.

Keywords: Radium-223; Barium-131; Calixarene

  • Poster
    23rd International Symposium on Radiopharmaceutical Sciences (ISRS 2019), 26.-31.05.2019, Peking, China
  • Open Access Logo Abstract in refereed journal
    Journal of Labelled Compounds and Radiopharmaceuticals 62(2019), S261

Publ.-Id: 29045

A multiscale approach simulating generic pool boiling

Höhne, T.; Lucas, D.

The paper presents an application of the GENTOP model for phase transfer and discusses the sub-models used. Boiling of a heated surface under atmospheric conditions is simulated by the multi-field CFD approach. Sub-cooled water in a generic pool is heated up first in the near wall region leading to the generation of small bubbles. Further away from the bottom wall larger bubbles are generated by coalescence and evaporation. The CFD simulation bases on the recently developed GEneralized TwO Phase flow (GENTOP) concept. It is a multi-field model using the Euler-Euler approach and it allows the consideration of different local flow morphologies including transitions between them. Small steam bubbles are handled as dispersed phases while the interface of large gas structures is statistically resolved. The GENTOP sub-models need a constant improvement and separate, intensive validation effort using CFD grade experiments. Recently, a bubble dynamics model inside the heat partitioning approach has been developed and will be applied in GENTOP in future.

Keywords: multi-phase; boiling; GENTOP; multi-scale; CFD

  • Lecture (Conference)
    18th International Topical Meeting on Nuclear Reactor Thermal Hydraulics (NURETH-18), 18.-23.08.2019, Portland, USA
  • Contribution to proceedings
    18th International Topical Meeting on Nuclear Reactor Thermal Hydraulics (NURETH-18), 18.-23.08.2019, Portland, USA
  • Open Access Logo Nuclear Science and Engineering 194(2020)10, 859-872
    Online First (2020) DOI: 10.1080/00295639.2020.1764265


Publ.-Id: 29043

Energy relaxation and electron phonon coupling in laser heated solids

Vorberger, J.; Butcher, T. A.

density functional theory based description of electron phonon coupling for energy relaxation in laser heated solids

Keywords: warm dense matter; energy relaxation; temperature relaxation; electron-phonon coupling; laser heating

  • Open Access Logo Contribution to proceedings
    39th International Workshop on High Energy Density Physics with Intense Ion and Laser Beams, 27.01.-01.02.2019, Hirschegg, Austria


Publ.-Id: 29042

Multiphase CFD Modelling: State-of-the-art applications in Energy related Industrial Applications

Höhne, T.

Two-phase flows occur in many industrial processes. Reliable predictions on flow characteristics are necessary for the design, process optimization and safety analysis of related apparatuses and processes. Experimental investigations are expensive and in most cases not transferable to modified geometries or different scales and flow conditions. For this reason there is a clear requirement for numerical tools. Due to the 3D nature of flows and the importance of turbulence in most cases this means a strong need for reliable 3D CFD-tools rather than 1D system codes or simplified correlations. The general aim is to provide simulation tools for the design, optimization and safety analyses of medium and large scale applications in which multiphase flows are involved. Such tools can contribute to improve the efficient use of energy and resources (e.g. in chemical engineering and oil industries) and to guarantee the safe operation (especially nuclear safety) – provided that they are predictive. Since large scale applications are considered such as chemical reactors or components of the cooling system of a nuclear power plant the Euler-Euler two- or multi fluid model is the base for the development. Presently the predictive capabilities for basic hydrodynamics are restricted due to limitations of the closure models. For this reason one focus of our multiphase flow research is the improvement of the closures first for adiabatic flow modelling but also phase transfer, chemical reactions etc. have to be considered. A second focus is to establish modelling frameworks as iMUSIG, AIAD and GENTOP to allow a proper consideration of the local physical phenomena. These activities will help to improve the CFD code capabilities in energy related industrial applications.

Keywords: CFD; Multiphase; Fluid Dynamics; HZDR; AIAD; GENTOP

  • Invited lecture (Conferences)
    The 9th International Conference & Workshop REMOO–2019, 16.-18.04.2019, Hong Kong, China
  • Contribution to proceedings
    The 9th International Conference & Workshop REMOO–2019, 16.-18.04.2019, Hong Kong, China

Publ.-Id: 29041

Radium-doped BaSO4 Nanoparticles for Future Targeted Alpha Therapy

Reissig, F.; Pietzsch, H.-J.; Steinbach, J.; Mamat, C.

Targeted alpha therapy (TAT) is continually focused and discussed in radiopharmaceutical research [1]. By the combination of an alpha emitting radionuclide with a biological targeting unit, tumor cells can be affected very efficiently by inducing a high number of double strand breaks to the DNA. 223Ra and 224Ra are two alpha-emitting radionuclides with suitable half-lives for TAT. 223Ra in form of [223Ra]RaCl2 (Xofigo®) is the only EMA- and FDA-approved alpha-emitting radiopharmaceutical as well as the prime example for the working principle of TAT. Based on its calcimimetic behavior, radium is built into the bone structure. To exploit the therapeutic potential of alpha emitters like 223Ra and 224Ra, novel targeting strategies and carrier systems have to be developed. Therefore, it is worth to examine alternative carriers like nanoparticles, using the principle of co-precipitation of Ra/BaSO4. By the combination of a therapeutic alpha-emitting radionuclide like 223Ra on the one hand and the diagnostically applicable barium radioisotope 131Ba on the other hand with nearly identical physical half-lives it is also possible pursue theragnostic approaches. Thus, our research aims at developing a simple method for the synthesis of small radiolabeled Ra/BaSO4 nanoparticles and testing further surface functionalization regarding the ability of constructing biological targeting moieties.

Keywords: Radium-224; Barium-131; Nanoparticle

  • Poster
    23rd International Symposium on Radiopharmaceutical Sciences (ISRS 2019), 26.-31.05.2019, Peking, China
  • Open Access Logo Abstract in refereed journal
    Journal of Labelled Compounds and Radiopharmaceuticals 62(2019), S265

Publ.-Id: 29040

Calixarene-based ligands for Radium and Barium

Bauer, D.; Reissig, F.; Pietzsch, H.-J.; Steinbach, J.; Mamat, C.

Due to their high biological effectiveness and suitable half-lives, there is increased interest in using the radionuclides radium-223 and radium-224 for radiopharmaceutical applications. Xofigo ([223Ra]radium chloride) is a bone-seeking, alpha-emitting radiopharmaceutical with EMA and FDA approval. It is used to treat bone metastasis of castrate-resistant prostate cancer. To expand the possible applications for these promising radionuclides, it is necessary to stably bind the radionuclide within a chelator. Therefore, calixarene-based ligands have been synthesized, which show encouraging affinities to radium ions. In our recent studies, we have already presented the high potential of these ligands. Since radium and barium have similar chemistry, and therefore comparable affinities to our ligands, it is possible to create a matched pair for theragnostic approaches. The radionuclide barium-131 has a suitable physical half-life for therapeutic applications and the potential of being a SPECT nuclide.

Keywords: Radium-224; Barium-131; Calixarene

  • Poster
    11th International Symposium on Targeted-Alpha-Therapy, 01.-06.04.2019, Ottawa, Kanada
  • Open Access Logo Abstract in refereed journal
    Journal of Medical Imaging and Radiation Sciences 50(2019)1, S39
    DOI: 10.1016/j.jmir.2019.03.118

Publ.-Id: 29039

Interobserver variability of image-derived arterial blood SUV in whole-body FDG PET

Hofheinz, F.; Maus, J.; Zschaeck, S.; Rogasch, J.; Schramm, G.; Oehme, L.; Apostolova, I.; Kotzerke, J.; van den Hoff, J.

Background: Today, the standardized uptake value (SUV) is essentially the only means for quantitative evaluation of static [18 F-]fluorodeoxyglucose (FDG) positron emission tomography (PET) investigations. However, the SUV approach has several well-known shortcomings which adversely affect the reliability of the SUV as a surrogate of the metabolic rate of glucose consumption. The standard uptake ratio (SUR), i.e., the uptake time-corrected ratio of tumor SUV to image-derived arterial blood SUV, has been shown in the first clinical studies to overcome most of these shortcomings, to decrease test-retest variability, and to increase the prognostic value in comparison to SUV. However, it is unclear, to what extent the SUR approach is vulnerable to observer variability of the additionally required blood SUV (BSUV) determination. The goal of the present work was the investigation of the interobserver variability of image-derived BSUV.

Methods: FDG PET/CT scans from 83 patients (72 male, 11 female) with non-small cell lung cancer (N = 46) or head and neck cancer (N = 37) were included. BSUV was determined by 8 individuals, each applying a dedicated delineation tool for the BSUV determination in the aorta. Two of the observers applied two further tools. Altogether, five different delineation tools were used. With each used tool, delineation was performed for the whole patient group, resulting in 12 distinct observations per patient. Intersubject variability of BSUV determination was assessed using the fractional deviations for the individual patients from the patient group average and was quantified as standard deviation (SDis ), 95% confidence interval, and range. Interobserver variability of BSUV determination was assessed using the fractional deviations of the individual observers from the observer-average for the considered patient and quantified as standard deviations (SDp , SDd ) or root mean square (RMS), 95% confidence interval, and range in each patient, each observer, and the pooled data respectively.

Results: Interobserver variability in the pooled data amounts to RMS = 2.8% and is much smaller than the intersubject variability of BSUV (SDis = 16%). Averaged over the whole patient group, deviations of individual observers from the observer average are very small and fall in the range [− 0.96, 1.05]%. However, interobserver variability partly differs distinctly for different patients, covering a range of [0.7, 7.4]% in the investigated patient group.

Conclusion: The present investigation demonstrates that the image-based manual determination of BSUV in the aorta is sufficiently reproducible across different observers and delineation tools which is a prerequisite for accurate SUR determination. This finding is in line with the already demonstrated superior prognostic value of SUR in comparison to SUV in the first clinical studies.

Keywords: PET; FDG; Quantification; SUV; SUR; Blood SUV

Publ.-Id: 29038

Flexible IGZO TFTs and their Suitability for Space Applications

Costa, J. C.; Pouryazdan, A.; Panidi, J.; Spina, F.; Anthopoulos, T.; Liedke, M. O.; Schneider, C.; Wagner, A.; Münzenrieder, N.

In this paper, Low Earth Orbit radiation, temperature and magnetic field conditions are mimicked to investigate the suitability of flexible Indium Gallium Zinc Oxide transistors for lightweight space wearables. Such wearable devices could be incorporated into spacesuits as unobtrusive radiation detectors or physiological monitors. Due to the harsh environment to which these space wearables would be exposed, they have to be able to withstand high radiation doses, low temperatures and magnetic fields. For this reason, the impacts of high energetic electron irradiation with fluences up to 1E12 e−/cm2, low operating temperatures down to 78K and magnetic fields up to 11mT are investigated. This simulates 278 h in Low Earth Orbit. The threshold voltage and mobility of transistors that were exposed to e- irradiation are found to shift by +(0.09 +- 0.05)V and (0.6 +- 0.5) cm 2 V−1 s−1. Subsequent low temperature exposure resulted in additional shifts of +0.38V and -5.95 cm2 V−1 s−1 for the same parameters. These values are larger than the ones obtained from non irradiated reference samples. In addition, the performance of the devices was observed not to be significantly affected by the magnetic fields. Finally, a Cascode amplifier presenting a voltage gain of 10.3 dB and a cutoff frequency of 1.2 kHz is demonstrated after the sample had been irradiate, cooled down and exposed to the magnetic fields. If these notions are considered during the systems’ design, these devices can be used to unobtrusively integrate sensor systems into space suits.

Keywords: Flexible electronics; Wearables; Amorphousnoxides; Thin film transistors; Space applications

Publ.-Id: 29037

Fifteen Years of Radionuclide Research at the KIT Synchrotron Source in the Context of the Nuclear Waste Disposal Safety Case

Rothe, J.; Altmaier, M.; Dagan, R.; Dardenne, K.; Fellhauer, D.; Gaona, X.; González-Robles Corrales, E.; Herm, M.; Kvashnina, K.; Metz, V.; Pidchenko, I.; Schild, D.; Vitova, T.; Geckeis, H.

For more than 120 years, systematic studies of X-ray interaction with matter have been the basis for our understanding of materials—both of natural or man-made origin—and their structure-function relationships. Beginning with simple radiographic imaging at the end of the 19th century, X-ray based analytical tools such as X-ray diffraction, X-ray fluorescence and photoemission or X-ray absorption techniques are indispensable in almost any field of chemical and material sciences—including basic and applied actinide and radionuclide studies. The advent of dedicated synchrotron radiation (SR) sources in the second half of the last century has revolutionized the analytical power of X-ray probes, while—with increasing number of SR facilities—beamline instrumentation followed a trend towards increasing specialization and adaption to a major research topic. The INE-Beamline and ACT station at the KIT synchrotron source belong to the exclusive club of a few synchrotron beamline facilities—mostly located in Europe—dedicated to the investigation of highly radioactive materials. Since commissioning of the INE-Beamline in 2005, capabilities for synchrotron-based radionuclide and actinide sciences at KIT have been continuously expanded, driven by in-house research programs and external user needs.

Publ.-Id: 29035

Metallgewinnung durch Mikrobiologie – Biologisch assistierte Prozesse in der Rohstofftechnologie

Lederer, F.

Der Rohstoffsektor ist geprägt von enormem Materialbedarf für die Entwicklung und Produktion neuer High-Tech Produkte. Neben der Optimierung von Bergbauprozessen zur Gewinnung von primären Rohstoffen fokussiert das Helmholtz-Institut Freiberg für Ressourcentechnologie die Vision der Kreislaufwirtschaft. Diese setzte neben dem Schwerpunkt Nachhaltigkeit im Hinblick auf Produktdesign, Produktion, Verteilung, Konsum, Verwendung, Reparatur und Sammlung vor allem auf das Recycling von Wertstoffen.
Mikrobiologisch assistierte Recyclingprozesse zur Rückgewinnung von Wertstoffen aus Elektronikschrott und Bergbauresthalden sowie innovative und umweltfreundliche Lösungen für die Ressourcensicherung standen im Fokus der 29. Jenaer Industriegespräche der DPG.
Themenschwerpunkte des Vortrages waren Interaktionen von Mikroorganismen mit Metallen, das biotechnologische Potential neuer Ressourcentechnologien, Grenzen überwindende Bioflotation, die Metallgewinnung mittels Siderophoren, Evolution im Reagenzglas sowie Biokollektoren für das Recycling von Wertstoffen aus Elektroschrott.

  • Invited lecture (Conferences)
    29. Jenaer Industriegespräche der DPG, 20.03.2019, Jena, Deutschland

Publ.-Id: 29034

Consolidative thoracic radiotherapy in stage IV small cell lung cancer: Selection of patients amongst European IASLC and ESTRO experts

Putora, P. M.; Glatzer, M.; de Ruysscher, D.; Faivre-Finn, C.; Belderbos, J.; Besse, B.; Blackhall, F.; Califano, R.; Cappuzzo, F.; de Marinis, F.; Dziadiuszko, R.; Felip, E.; Früh, M.; Garrido, P.; Le Pechoux, C.; Mcdonald, F.; Nestle, U.; Novello, S.; Brien, M. O.; Paz Ares, L.; Peeters, S.; Pöttgen, S.; Ramella, S.; Reck, M.; Troost, E. G. C.; van Houtte, P.; Westeel, V.; Widder, J.; Mornex, F.; Slotman, B. J.

Background: The role of consolidative thoracic radiotherapy (TRT) in stage IV small cell lung cancer (SCLC) is not uniformly accepted. Methods: We obtained a list of 13 European medical oncologists from the International Association for the Study of Lung Cancer (IASLC) and 13 European radiation oncologists from the European Society for Therapeutic Radiation Oncology (ESTRO). The strategies in decision making for TRT in stage IV SCLC were collected. Decision trees were created representing these strategies. Frequencies of recommending TRT were analysed for various parameter combinations based on the objective consensus methodology. Results: The factors associated with the recommendation for TRT included fitness of the patient, limited extrathoracic tumour burden, initial bulky thoracic disease and response to chemotherapy. The highest consensus for TRT was in fit patients with limited extrathoracic tumour burden and initial bulky disease with either a complete extrathoracic response or partial thoracic response (92% recommend TRT). For these patients the recommendations were the same for medical and radiation oncologists. In the setting of partial response (intra- and extra-thoracically) without initial bulky thoracic disease radiation oncologists were more likely to recommend TRT than medical oncologists. For unfit patients or for patients with poor overall response to chemotherapy, the majority did not recommend TRT. Conclusion: European radiation and medical oncologists specializing in lung cancer recommend TRT in selected patients with stage IV SCLC and restrict its use primarily to fit patients who responded to chemotherapy with limited extrathoracic tumour burden.

Keywords: ESTRO; Expert opinion; IASLC; Small cell lung cancer; Stage IV; Thoracic radiotherapy

Publ.-Id: 29033

Repeat FMISO-PET imaging weakly correlates with hypoxia-associated gene expressions for locally advanced HNSCC treated by primary radiochemotherapy

Löck, S.; Linge, A.; Seidlitz, A.; Bandurska-Luque, A.; Nowak, A.; Gudziol, V.; Buchholz, F.; Aust, D. E.; Baretton, G. B.; Zöphel, K.; Steinbach, J.; Kotzerke, J.; Overgaard, J.; Zips, D.; Krause, M.; Baumann, M.; Troost, E. G. C.

Background: Hypoxia is an important factor of tumour resistance to radiotherapy, chemotherapy and potentially immunotherapy. It can be measured e.g. by positron emission tomography (PET) imaging or hypoxia-associated gene expressions from tumour biopsies. Here we correlate [ 18 F]fluoromisonidazole (FMISO)-PET/CT imaging with hypoxia-associated gene expressions on a cohort of 50 head and neck squamous cell carcinoma (HNSCC) patients and compare their prognostic value for response to radiochemotherapy (RCTx). Methods: FMISO-PET/CT images of 50 HNSCC patients were acquired at four time-points before and during RCTx. For 42 of these patients, hypoxia-associated gene expressions were evaluated by nanoString technology based on a biopsy obtained before any treatment. The FMISO-PET parameters tumour-to-background ratio and hypoxic volume were correlated to the expressions of 58 hypoxia-associated genes using the Spearman correlation coefficient ρ. Three hypoxia-associated gene signatures were compared regarding their correlation with the FMISO-PET parameters using their median expression. In addition, the correlation with tumour volume was analysed. The impact of both hypoxia measurement methods on loco-regional tumour control (LRC) and overall survival (OS) was assessed by Cox regression. Results: The median expression of hypoxia-associated genes was weakly correlated to hypoxia measured by FMISO-PET imaging (ρ ≤ 0.43), with higher correlations to imaging after weeks 1 and 2 of treatment (p < 0.001). Moderate correlations were obtained between FMISO-PET imaging and tumour volume (ρ ≤ 0.69). Prognostic models for LRC and OS based on the FMISO-PET parameters could not be improved by including hypoxia classifiers. Conclusion: We observed low correlations between hypoxia FMISO-PET parameters and expressions of hypoxia-associated genes. Since FMISO-PET showed a superior patient stratification, it may be the preferred biomarker over hypoxia-associated genes for stratifying patients with locally advanced HNSCC treated by primary RCTx.

Keywords: FMISO-PET; Gene signature; Hypoxia; Locally advanced HNSCC; Radiochemotherapy

Publ.-Id: 29032

Combining magnetic forces for contactless manipulation of fluids in microelectrode-microfluidic systems

Hähnel, V.; Khan, F. Z.; Mutschke, G.; Cierpka, C.; Uhlemann, M.; Fritsch, I.

A novel method to drive and manipulate fluid in a contactless way in a microelectrode-microfluidic system is demonstrated by combining the Lorentz and magnetic field gradient forces. The method is based on the redox-reaction [Fe(CN)6]3−/[Fe(CN)6]4− performed in a magnetic field oriented perpendicular to the ionic current that crosses the gap between two arrays of oppositely polarized microelectrodes, generating a magnetohydrodynamic flow. Additionally, a movable magnetized CoFe micro-strip is placed at different positions beneath the gap. In this region, the magnetic flux density is changed locally and a strong magnetic field gradient is formed. The redox-reaction changes the magnetic susceptibility of the electrolyte near the electrodes, and the resulting magnetic field gradient exerts a force on the fluid, which leads to a deflection of the Lorentz force-driven main flow.
Particle Image Velocity measurements and numerical simulations demonstrate that by combining the two magnetic forces, the flow is not only redirected, but also a local change of concentration of paramagnetic species is realized.

Keywords: microfluidics; electrochemistry; redox-reaction; magnetic field; Lorentz force; magnetic gradient force; flow control

  • Open Access Logo Scientific Reports 9(2019), 5103
    DOI: 10.1038/s41598-019-41284-0
  • Lecture (Conference)
    11th International PAMIR International Conference - Fundamental and Applied MHD, 01.-05.07.2019, Reims, Frankreich

Publ.-Id: 29031

Avoided energy cost of producing minerals: The case of iron ore

Reuter, M. A.; Palacios, J.-L.; Fernandes, I.; Abadias, A.; Valero, A.; Valero, A.

There is growing concern about the decline of the ore grade in mines and the increased energy usage for processing and refining metals. In the limit, where no concentrated deposits exist, minerals must be obtained from bare rock. A method for quantitatively assessing the “free bonus” granted by nature in providing concentrated minerals in mines and thus assessing the quality of the different resources is estimating how much energy is needed to concentrate the minerals, as they are already in mines, from bare rock. This bonus granted by nature reduces the costs of human mining and metallurgical processes, as well as the mining effort required of future generations. In this study, the concentration of high-iron-content minerals in common rocks was investigated via a computational model developed using the HSC software. As expected, the range of results for the specific energy for the concentration of iron from common rocks was considerably higher than the energy required by modern processes. This reveals the need to value current iron deposits and the challenge of developing sustainable methods of metal production to satisfy the needs of the present and future generations.

Keywords: Energy consumption; Exergy replacement cost; Iron; Metallurgy; Mining; Thanatia

Publ.-Id: 29030

Einfluss polymerer Zementadditive auf die Mobilität von Radionukliden unter Nahfeldbedingungen eines Endlagers

Lippold, H.; Becker, M.; Schymura, S.

Zementmaterialien, die im Endlagersystem als Bau- und Versatzstoff verwendet werden, enthalten polymere Fließmittel (Superplasticizer) mit komplexierenden Eigenschaften. Insbesondere in Niedrig-pH-Zement kann eine teilweise Persistenz nicht ausgeschlossen werden [1]. Bei Freisetzung durch Laugungsprozesse nach Wasserzutritt besteht die Möglichkeit, dass Adsorptionsbarrieren für Radiometalle durch Komplexbildung unterwandert werden [2, 3]. Die entsprechenden Randbedingungen (pH-Wert, Elektrolytgehalt) sind zu identifizieren.

Die Komplexbildung von Eu(III) (Actinid-Analogon) mit einem kommerziellen Superplasticizer auf Polycarboxylatether-Basis (MasterGlenium® 51, BASF) wurde mittels Ultrafiltration und 152Eu als Radiotracer konzentrationsabhängig vermessen und auf der Grundlage des Ladungsneutralisationsmodells [4] mit Bezug auf den Carboxylgruppengehalt parametrisiert. Bei geringer Ionenstärke besteht demnach ein hohes Mobilisierungspotential. Die für Zementsysteme typischen hohen Elektrolytgehalte schränken den Effekt allerdings stark ein. Die Auswirkung des Plasticizers auf das Adsorptionsverhalten von Eu(III) an Ca-Bentonit als Puffermaterial wurde in Gegenwart von NaCl und CaCl2 (bis 4 mol/L) unter CO2-Ausschluss im pH-Bereich 9 - 13 untersucht. Die Mobilität des Metalls wird bereits bei moderaten Ionenstärken ausschließlich durch den Elektrolyteffekt bestimmt, eine Komplexbildung also völlig unterbunden. Somit ist aufgrund des chemischen Milieus im Endlagernahfeld selbst im Falle einer Freisetzung der intakten Polymere nicht von Carrier-Effekten auszugehen.

[1] M. A. Glaus, L. R. Van Loon, Nagra Technical Report 03-09, 2004.
[2] M. Dario et al., SKB Technical Report TR-04-04, 2004.
[3] A. J. Young, Dissertation, Loughborough University, 2012.
[4] J. I. Kim, K. R. Czerwinski, Radiochim. Acta 1996, 73, 5.

  • Poster
    Jahrestagung der GDCh-Fachgruppe Nuklearchemie, 25.-27.09.2019, Dresden, Deutschland

Publ.-Id: 29029

Doping of silicon nanowires by ion implantation and flash lamp annealing

Berencen, Y.; Prucnal, S.; Wang, M.; Rebohle, L.; Helm, M.; Zhou, S.; Skorupa, W.

In this work, we report on non-equilibrium processing for controlled doping of Si/SiO2 core/shell nanowires with shallow- and deep-level dopants below and above their equilibrium solid solubility. In detail, the shallow-level dopants B and P as well as the deep-level dopant Se was implanted, followed by millisecond flash lamp annealing. In case of amorphization upon high-fluence implantation, recrystallization takes place via a bottom-up template-assisted solid phase epitaxy. Non-equilibrium Se concentrations lead to the formation of an intermediate band in Si which in turn causes a room-temperature sub-band gap photoresponse of the nanowire when configured as a photoconductor device [1]. Alternatively, the formation of a cross-sectional p-n junction is demonstrated by co-implanting P and B in individual nanowires at different depth along the NW core.
[1] Y. Berencén, et al. Adv. Mater. Interfaces 2018, 1800101

Keywords: doping; nanowires; semiconductor; silicon; ion implantation; flash lamp annealing

  • Lecture (Conference)
    44. Treffen der Nutzergruppe Heißprozesse und RTP, 03.04.2019, Erlangen, Deutschland

Publ.-Id: 29028

Evaluierung der Tracking Genauigkeit eines Niedrigfeld MR-LINACs mittels eines 4D MRT Bewegungsphantoms

Schneider, S.; Dolde, K.; Rothlübbers, S.; Jenne, J.; Spindeldreier, K.; Pfaffenberger, A.; Hoffmann, A.; Klüter, S.

Mit der Entwicklung von hybriden Magnetresonanz-geführten Linearbeschleunigern (MR-LINAC) wurde die Möglichkeit der MR-Echtzeitbildgebung während der Strahlentherapie klinische Realität. Gerade Patienten mit bewegten Tumoren könnten davon profitieren, da die Tumorbewegung durch Gating oder Tracking Verfahren kompensiert werden kann. Ziel dieser Studie war die Evaluierung der Genauigkeit der implementierten online Echtzeit Tracking-Verfahren eines 0.35 T MR-LINAC, sowie der Vergleich zu alternativen offline Tracking-Algorithmen Verfahren.

Material & Methoden
Ein MRT-Bewegungsphantom wurde mit klinisch verwendeter sagittaler cine-MR Bildgebung gescannt. Das bewegbare Hoch-Kontrast Target des Phantoms vollführte dabei verschiedene sinusförmige 1D, 2D, und 3D Trajektorien unterschiedlicher Amplituden (4.5-40 mm) bei einer Frequenz von 0.2 Hz. Die Genauigkeit der im MR-Scanner implementierten, auf deformierbarer Registrierung basierenden, online Tracking Verfahren (TM-1, TM-2) wurde evaluiert. Diese wurde mit einer offline Schwellenwert-basierten Tracking Analyse (TM-3) und einem Echtzeit-fähigen Particle Filter Algorithmus basierenden Tracking Verfahren verglichen. Damit wurde die erreichbare Genauigkeit der Tracking Verfahren untersucht, die die 2D cine MR-Bildgebung prinzipiell ermöglicht.

Die online Tracking Methoden TM-1 und TM-2 beschrieben die vorgegebene Bewegung mit einer durchschnittlichen Abweichung der Schwerpunktsbewegung von der vorgegebenen Trajektorie von Δ_mittelTM-1 ≤ 1.5 mm und Δ_mittelTM-2 ≤ 2.7 mm und einer maximalen Abweichung von Δ_maxTM-1 ≤ 5.1 mm und Δ_maxTM-2 ≤ 5.4 mm. TM-3 resultierte in Δ_mittelTM-3 ≤ 0.4 mm und Δ_maxTM-3 ≤ 3.1 mm, während TM-4 die Bewegung teilweise präziser akkurater beschrieb mit Δ_meanTM-4 ≤ 0.4 mm und Δ_maxTM-4 ≤ 2.4 mm.

Wenn auch das klinisch verwendete Tracking Verfahren TM-1 für Gating zufriedenstellende Genauigkeiten erreicht, erlaubt die Bildgebung des Hoch-Kontrast Targets des Phantoms am MR-LINACs höhere Genauigkeiten. Mit entsprechend entwickelten Tracking-Algorithmen lässt sich diese Genauigkeit prinzipiell auch in Echtzeit erreichen.

Keywords: MR-Linac; 4D MRI Phantom; Tracking

  • Poster
    50. Jahrestagung der Deutschen Gesellschaft für Medizinische Physik (DGMP) e. V., 18.-21.09.2019, Stuttgart, Deutschland

Publ.-Id: 29027

Ultrasonic flow measurements in liquid metal flows with partial solidification

Franke, S.; Räbiger, D.; Eckert, S.

The monitoring of the flow rate is an inherent part of process control in all technical large-scale plants to guarantee process stability and safety. It is particularly important for nuclear applications. In the case of a liquid metal coolant in addition, the control of the aggregate state is important.
The use of ultrasound techniques opens an attractive opportunity to measure both the fluid velocity by evaluating the Doppler phase shift and the phase boundary by the detection of the reflection signal from the interface. In addition, the measuring principle enables a noninvasive implementation of the measuring technique. A test facility is necessary to qualify the measuring technique for real applications.
In this study a new LBE experimental facility has been designed and constructed. The setup enables to control the temperature and the fluid flow in the liquid. Further a partial solidification can be induced. The liquid metal vessel is equipped with ten ports for ultrasonic probes. These ports allow for testing the ultrasound measuring principle for different conditions. It was demonstrated that the ultrasonic sensors can be operated up to 200°C at the piezo element. First measuring results demonstrate the potential of ultrasound measuring techniques for monitoring liquid metal applications.

  • Lecture (Conference)
    SESAME International Workshop, 19.-21.03.2019, Petten, Netherlands
  • Contribution to proceedings
    SESAME International Workshop, 19.-21.03.2019, Petten, Netherlands
    SESAME International Workshop

Publ.-Id: 29026

Probing charged lepton flavor violation with the Mu2e experiment

Mueller, S. E.; Ferrari, A.

The Mu2e experiment, currently under construction at the Fermi National Accelerator Laboratory near Chicago, will search for the neutrinoless conversion of muons to electrons in the field of an aluminum nucleus. In the Standard Model, this process, which violates charged lepton flavor, is highly suppressed and therefore undetectable. However, scenarios for physics beyond the Standard Model predict small but observable rates. The Mu2e experiment aims at a sensitivity four orders of magnitude better than existing experiments. This is achieved by a rigorous control of all backgrounds that could mimic the monoenergetic conversion electron.

At HZDR, we use the ELBE radiation facility to study radiation hardness and performance of components for the Mu2e calorimeter and contribute with Monte Carlo simulations to the understanding of the optimal configuration for the detector that will monitor the rate of stopped muons in the aluminum target. Additional simulations are performed for both the pion production target and the muon stopping target.

In the presentation, the design and status of the Mu2e experiment will be presented, and results from the ELBE beamtimes and the simulation studies will be given.

Keywords: Mu2e; CLFV; ELBE

  • Lecture (Conference)
    Spring Meeting DPG, 22.03.2019, Muenchen, Deutschland

Publ.-Id: 29025

Composition and Structure of Surface Oxides on Press-Hardened Hot-Dip Galvanized Steel

Gaderbauer, W.; Arndt, M.; Steck, T.; Klingner, N.; Faderl, J.; Groiß, H.

Zink-coated press hardened steel (PHS) is due to its extremely high tensile strength and its excellent corrosive protection indispensable for structural elements in modern automotive applications. Different studies clarify the resulting microstructure of the Zn-coating after press hardening [1] of such steel parts. Also, the uppermost surface oxide layer, which can be influenced by steel matrix alloy elements, has a significant impact on the processing properties like coating or welding.
In this study, we investigated these surface oxide layers for alloy compositions of four different PHS systems with scanning and conventional transmission electron microscopy (TEM), Auger electron spectroscopy (AES) and helium ion microscopy (HIM). The complex and porous oxide-layers were stabilized by epoxy before the preparation of cross-sections and TEM-lamellae by focused ion beam milling.
The main oxides on top of the original thin Al2O3 layer, originating from the primary galvanizing process, could be determined with energy dispersive X-ray spectroscopy (EDX), selected area diffraction and AES as Zn-oxides and (Mn,Zn)Mn2O4 spinel (Fig. 1a). Also noticeable was a varying, nanometre thick Cr enrichment at this Al2O3 layer (Fig. 1b), which depends strongly on the steel alloy. Further experiments with secondary mass spectrometry (ToF-SIMS) attached to a HIM [2] allowed reliable distinguishing between ZnO and Zn(OH)2 (Fig. 2c), which are both present in our oxide layers.
Thus, we could show an influence of different steel alloy elements on the final oxide structure after press hardening. The formation of spinel is triggered by Mn, which is transported with the Zn above the Al2O3 layer, which itself is a trap for Cr, leading to a coverage of it with Cr-oxides.

Figure 1. a) AES Mapping. b) STEM-EDX Mapping c) ToF-SIMS Mapping

[1] H. Järvinen et al, Surface and Coatings Technology 352 (2018), 378-391.
[2] N. Klingner et al, Ultramicroscopy 198 (2019), 10-17.

The financial support by the Austrian Federal Ministry for Digital and Economic Affairs and the National Foundation for Research, Technology and Development in the frame of the CDL for nanoscale phase transformations is gratefully acknowledged.

  • Lecture (Conference)
    9th Austrian Society for Electron Microscopy workshop, 25.-26.04.2019, Graz, Österreich

Publ.-Id: 29024

Entwicklung einer Positionierhilfe für die Bestrahlung von Weichgewebssarkomen des Unterarms in einem ersten klinischen Prototyp der MR-integrierten Protonentherapie

Anders, P.; Karsch, L.; Hoffmann, A.

Die Machbarkeit von gleichzeitiger Protonentherapie und MR-Bildgebung wurde bereits durch die experimentelle Integration eines Niederfeld-MRTs in eine statische Protonenstrahlführung gezeigt[1].
Als nächster Schritt wurde der MR-Scanner in eine Pencil-Beam-Scanning Strahlführung integriert. Dieser Aufbau soll perspektivisch für eine erste Patientenbestrahlung an Weichgewebssarkomen des Unterarms genutzt werden. Da die geometrischen Randbedingungen im in-beam-MRT lediglich eine Bestrahlung im Sitzen mit seitlich ausgestrecktem Arm zulassen (Abb. 1), das Planungs-CT aber liegend mit über dem Kopf ausgestreckten Armen durchgeführt wird, ist eine neuartige Arm-Positionierhilfe notwendig. Der Beitrag zeigt deren Entwicklung anhand erster Ergebnisse.

Material & Methoden
Die Komponenten der Positionierhilfe (Armschiene, Griffe, Anschlagbolzen) wurden in der hauseigenen Werkstatt aus Polyurethan gefertigt. Diese können je nach Patientenanatomie ausgewechselt werden. Zur Evaluierung der Positioniergenauigkeit wurden wiederholt MRT-Bildserien eines Probanden einerseits in Bestrahlungsposition am 0,22T in-beam-MRT aufgenommen, andererseits an einem 3T-MRT aufgezeichnet (Abb. 2), um die Patientenposition während des Planungs-CTs zu simulieren. Mittels einer selbst programmierten Bildregistrierungssoftware wurden Positionsabweichungen bestimmt.

Die Positionierung des Arms konnte am 3T-MRT mit einer Unsicherheit von coronal sowie sagittal durchgeführt werden. Am 0,22T-MRT betrug die Unsicherheit coronal sowie transversal. Außerdem zeigte sich, dass die Armschiene für den Übergang aus der liegenden in die sitzende Position geeignet ist.

Eine Arm-Positionierhilfe für die erste Patientenbestrahlung von Weichgewebssarkomen des Unterarms an einem klinischen Prototyp für MR-integrierte Protonentherapie wurde entwickelt und evaluiert. Sie ermöglicht die Immobilisierung des Patientenarms sowohl in der üblichen Liegeposition des Planungs-CTs als auch in der aufgrund geometrischer Randbedingungen während der Bestrahlung nötigen Sitzposition im in-beam-MRT.

Keywords: Protonentherapie; MRT

  • Lecture (Conference)
    50. Jahrestagung der Deutschen Gesellschaft für Medizinische Physik (DGMP) e. V., 18.-21.09.2019, Stuttgart, Deutschland
  • Poster
    50. Jahrestagung der Deutschen Gesellschaft für Medizinische Physik (DGMP) e. V, 18.-21.09.2019, Stuttgart, Deutschland

Publ.-Id: 29022

Experimentelle Untersuchung der Strahlqualität für MR integrierten Protonentherapie

Gantz, S.; Schellhammer, S.; Smeets, J.; Hoffmann, A.

In ersten Untersuchungen zur Integration von MR-Bildgebung und Protonentherapie (MRiPT) konnte deren prinzipielle Machbarkeit an einer statischen Strahlführung gezeigt werden. Als weiterer Schritt zu einem klinischen Prototyp wurde nun der MR-Scanner mit einer Pencil-Beam-Scanning (PBS) Strahlführung integriert. Ziel dieser Arbeit ist die Charakterisierung der Strahlqualität im magnetischen Isozentrum des in-beam MR-Scanners.

Material & Methoden
Ein offener 0.22 T MR-Scanner (MrJ2200, ASG Superconductors) wurde nächstmöglich an eine horizontale PBS Protonenstrahlführung installiert. Strahlprofilmessungen wurden sowohl mit als auch ohne den MR-Scanner an der Position des magnetisches Isozentrums des MR-Scanners (39 cm strahlabwärts des nominalen PBS Isozentrums) durchgeführt. Strahlprofile wurden ohne MRT mithilfe eines Szintillatordetektors (Lynx, IBA Dosimetry) sowie im Untersuchungsfeld des MRT mittels radiochromen Filmen (GAFchromic EBT3, Ashland) vermessen (Abb. 1). Für beide Konfigurationen wurden für 3 verschiedene Protonenenergien(70, 125 und 220 MeV) Punktraster bis zur maximalen nominalen Feldgröße von 400x200 mm2 vermessen. Aus diesen Messungen wurden Spotgrößen, -position und -symmetrie sowie durch das Magnetfeld verursachte Strahlablenkungen und Feldverzerrungen ermittelt.

Spotgrößen mit und ohne Magnetfeld sind in Tabelle 1 zusammengefasst. Spotgrößen im Magnetfeld stimmen auf ±0.3 mm mit Ergebnissen ohne Magnetfeld überein. Die horizontale Strahlablenkung des Zentralspots beträgt 26, 19 und 15 mm für 70, 125 und 220 MeV. Durch das Magnetfeld tritt eine energieabhängige, trapezoidale Verzerrung des Bestrahlungsfeldes auf, mit vertikalen Höhenunterscheiden zwischen 10 und 16 mm, sowie einer energieabhängigen Rotation der achsfernen Punkte bis zu 45°.

Erstmals konnte die experimentelle Charakterisierung eines PBS-Strahls im Isozentrum des in-beam MR-Scanner erfolgen. Die Ergebnisse zeigen die Notwendigkeit weiterer präziser Messungen im Untersuchungsfeld des MR-Scanners, sowie für die Bestrahlungsplanung den Bedarf der Entwicklung eines dedizierten Strahlmodells unter Berücksichtigung des gesamten Magnetfeldes.

  • Lecture (Conference)
    50. DGMP Jahrestagung, 18.-21.09.2019, Stuttgart, Deutschland

Publ.-Id: 29021

Flüssigmetallbatterien als Option für elektrische Großspeicher

Nimtz, M.; Landgraf, S.; Personnettaz, P.; Weber, N.; Weier, T.

Der Bedarf an kostengünstigen Großspeichern für elektrische Energie wird zukünftig, bei zunehmendem Ausbau der erneuerbaren Energien, wachsen. Derzeit vorhandene Technologien (im wesentlichen Lithium-Ionen bzw. Blei-Säure Batterien) bieten bis in den Bereich von etwa 10 bis 30 MW bzw. MWh eine anwendungsbereite Speicherform.
Hauptanwendungsfeld ist hierbei zurzeit die Primärregelenergie, da dort vergleichsweise kleine Entladetiefen und nur wenige Vollzyklen auftreten. Ein Einsatz als Speicher im Stunden- oder gar Mehrtagesbetrieb kann von diesen Technologien jedoch meist nicht erbracht werden, da die Alterung der Zellen bei hohen Entladetiefen (ΔSOC > 50%) stark zunimmt und dementsprechend die Kapazität der Zellen bereits nach wenigen Jahren stark abnimmt.
Flüssigmetallbatterien [1] bieten eine Alternative zu den vorgenannten Technologien, wobei der Fokus hier auf dem Einsatz als Großspeicher (>>1 MWh) liegt. In Flüssigmetallbatterien liegen alle Aktivmaterialien in flüssiger Form vor. Alterungseffekte, die auf einer Schädigung oder auf der Degeneration der Elektrodenmaterialien beruhen, werden hier nicht erwartet. Prognostizierte Vollzyklenzahlen liegen im Bereich von 105 Vollzyklen, was die Flüssigmetallbatterien auch für den Einsatz abseits der Primärregelung interessant macht. Weitere Vorteile sind der einfache Aufbau, gute Skalierbarkeit und die leichte Wiederaufbereitung der verwendeten Materialien.
Der Beitrag stellt die Technologie, die Einsatzmöglichkeiten und Parameter sowie die Forschungsaktivitäten am Helmholtz-Zentrum Dresden-Rossendorf [2] vor. Schwerpunkt ist die Darstellung der neu entwickelten Software „LMB-System-Calculator“, welche eine integrierte Auslegung, Modellierung und Simulation von Flüssigmetallbatterien in Hinblick auf geometrische (siehe Abb. 1), elektrische und thermische Größen erlaubt.

Keywords: Flüssigmetallbatterie; Energiespeicher; Modellierung; Simulation; Liquid metal battery; energy storage; modelling; simulation

  • Lecture (Conference)
    51. Kraftwerkstechnisches Kolloquium, 22.-23.10.2019, Dresden, Deutschland
  • Contribution to proceedings
    51. Kraftwerkstechnisches Kolloquium, 22.-23.10.2019, Dresden, Deutschland
    Kraftwerkstechnik 2019 - Power PLant Technology, Freiberg: Saxonia, 978-3-934409-93-4, 677-686

Publ.-Id: 29019

An eurlerian-eulerian CFD approach to simulate the thermaohydrulics of piipes, channel or rod bundles: from onset of nucleate boiling to CHF

Ding, W.; Krepper, E.; Hampel, U.

The Eulerian-Eulerian computational fluid dynamics (CFD) approach is widely applied in the simulation of industrial scale thermal fluid dynamics problems, such as flow and heat transfer in fuel elements. However, the case dependency of submodels in the Eulerian-Eulerian CFD approach currently hampers its applicability. In order to reduce this dependency, a submodel to predict the bubble departure in both pool and flow boiling was developed in our group, which includes the impact of microlayer, thermal diffusion, condensation and force balance. Moreover, we also developed a new CHF- concept. It is currently based on correlations but we are continuously working on a transition to a fully physics-based model, which e.g. considers the dependency of boiling on the microlayer thickness, bubble base expansion speed and local shear stress. In order to implement the bubble dynamics model and CHF- model into the Eulerian-Eulerian CFD framework, a new cavity activation and heat partitioning model was developed, which is not only used for bubble nucleation but also connects the nucleate boiling and CHF- in one CFD approach. However, nucleation site density is strongly dependent on the surface properties, which is difficult to model without correlations.

Keywords: CFD; Wall boiling; CHF

  • Lecture (Conference)
    18th International Topical Meeting on Nuclear Reactor Thermal Hydraulics (NURETH-18), 18.-22.08.2019, Portland, USA

Publ.-Id: 29018

Critical heat flux as a mass flux dependent phenomenon: Theoretical analysis, experimental confirmation and further CFD application

Ding, W.; Geißler, T.; Krepper, E.; Hampel, U.

In this work, we report on a theoretical analysis and experimental investigations on critical heat flux (CHF) in subcooled flow boiling firstly. Commonly, CHF is considered as a local phenomenon. A validated CHF- concept recently developed in our group indicated that CHF may be initiated in two different ways, that is, locally and globally. We designed and conducted an experiment to verify this hypothesis. The experimental results agree well with the expectations from our CHF- modelling and confirm the two mechanisms. Following that, we continued to clarify the role of different parameters, such as channel orientation, channel length and hydraulic diameter. The new concept of CHF is useful to explain and predict CHF at conditions of low pressure and low fluid velocity. Further we applied this concept into an Euler-Euler computational multiphase fluid dynamics (CMFD) approach with wall boiling model which successfully predict the critical volume fraction under different conditions. The simulation results also had a good agreement with the corresponding experimental results.

Keywords: Critical heat flux; Boiling; CMFD

  • Invited lecture (Conferences)
    9th China-Korea Workshop on Nuclear Reactor Thermal-Hydraulics (WORTH-9), 15.-18.05.2019, Chongqing, China
  • Lecture (Conference)
    10th International Conference on Multiphase Flow, 19.-24.05.2019, Rio de Janeiro, Brazil

Publ.-Id: 29017

Fabrication and temperature-dependent electrical characterization of a C-shape nanowire patterned by a DNA origami

Bayrak, T.; Martinez-Reyes, A.; Ruiz-Arce, D. D.; Kelling, J.; Samano, E. C.; Erbe, A.

We introduce a method based on directed molecular self-assembly to manufacture C-shape gold nanowires which can serve as components of a metamaterial based on split-ring resonators. To this end, gold NPs are arranged in the desired shape on a DNA-origami template and enhanced to form a continuous wire through electroless deposition. C-shape nanowires with a size below 150nm on a SiO2/Si substrate are contacted with gold electrodes by means of electron beam lithography. Charge transport measurements of the nanowires show hopping, thermionic and tunneling transports at different temperatures in the 4.2K to 293K range. The different transport mechanisms indicated that the C-shape wires consist of metallic parts which are weakly coupled along the wire.

Publ.-Id: 29016

Pulse-front tilt in laser-plasma accelerators with short focal lengths

Steiniger, K.; Albach, D.; Bussmann, M.; Debus, A.; Kluge, T.; Loeser, M.; Pausch, R.; Siebold, M.; Zeil, K.; Schramm, U.

Laser ion accelerators utilize high-power laser pulses in tight-focusing geometries to provide pulsed, high-intensity ion beams. Efficient capturing, transport and application of these beams is an ongoing effort which depends on precise knowledge of the accelerated ion distribution's properties and how to control these. For example, it is known that the propagation direction of the accelerated ions can be controlled by tilting the driving laser pulse-front. Since laser pulse-front tilts can be present accidentally, for example by a small misalignment of the compressor gratings in a chirped-pulse amplification system, knowledge of the scaling of the pulse-front tilt at a target position is desired. The talk gives relations for pulse-front orientation dependent on setup parameters and identifies regimes were pulse-front tilt has a sizable impact.

Keywords: Pulse-front tilt; high-power laser

  • Lecture (Conference)
    DPG-Frühjahrstagung, 17.-22.03.2019, München, Deutschland

Publ.-Id: 29015

Flüssigmetallbatterien als Großspeicher - Technologie, Scale-Up und Optionen zur Sektorkopplung

Nimtz, M.

Es werden die grundsätzlichen Eigenschaften von Flüssigmetallbatterien beschrieben sowie Methoden und Ergebnisse zum Scale-Up vorgestellt. Des weiteren werden Funktionsweise und Anwendung der LMB-System-Calculator Software erläutert sowie Anwendungsoptionen für Flüssigmetallbbatterien, insbesondere bei der Sektorkoppelung vorgestellt.

Basic properties of Liquid Metal Batteries are described and methods and results for scale-up calculations are presented.
Also, functioning and usage of the LMB-System-Calculator software are discussed and options for the operation of Liquid Metal Batteries, especially for the sector-coupling are presented.

Keywords: LMB; Flüssigmetallbatterien; Scale-Up; Speicher; Sektorkoppelung; LMB; liquid metal battery; scale-up; storage; sectro-coupling

  • Lecture (others)
    Energie System 2050 Forschungsthema 1, 1. Workshop 2019, 19.-20.03.2019, Karlsruhe, Deutschland

Publ.-Id: 29014

Chemistry and accelerator mass spectrometry – A life happily ever after?

Merchel, S.

Accelerator mass spectrometry (AMS) is the most sensitive analytical method to measure long-lived radionuclides. The detection limits are generally several orders of magnitude better, i.e. as low as 10-16 (radionuclide/stable nuclide), than any other mass spectrometry or decay counting method. AMS needs smaller sample sizes and measurements are finished within a few minutes to hours.

However, it is often forgotten that research projects applying AMS start with taking appropriate samples, followed by labour- and cost-intensive sample preparation. The goal can easily be described as “making the big samples (up to several kg’s) to fit in an AMS target holder (< 10 mg)”. This includes getting rid of the matrix and the troublesome isobars. By technical improvements of AMS leading to lower detection limits or better mass-and-element discrimination, sample masses can be reduced to gram-quantities instead of kg’s allowing easier, faster, and cheaper chemistry. Recent AMS developments also address very efficiently isobar elimination.

Nevertheless, some samples can contain different sources of the radionuclide-of-interest such as ¹⁰Be produced in the Earth’s atmosphere polluting the ¹⁰Be of interest produced in-situ in quartz. Hence, in this case chemistry is inevitable for cleaning the samples from the contamination. Another “mission” of chemistry might be the reduction of corresponding stable nuclides, e.g. 35,37Cl, ²⁷Al, natFe by preceding cleaning or by gentle leaching to enhance the radionuclide/stable nuclide ratio or to minimize interfering nuclear reactions such as thermal-neutron capture on ³⁵Cl. When applying isotope-dilution AMS to simultaneously determine the natCl content of a sample, which is an absolute requirement for surface exposure dating of Ca- or K-rich minerals, chemical sample preparation is also mandatory.

As the majority of research projects involving AMS is of true interdisciplinary character, knowledge of sample preparation is usually passed-on to (young) non-chemists. These are trained learning-by-doing to perform the chemical preparation of their own samples. Therefore, the development of “routine” AMS sample preparation needs to have a strong focus on safety and easy-to-be-trained aspects with the least opportunity for failure.

In conclusion, although new AMS technical developments for isobar suppression like the laser-negative ion interaction system at VERA promise to reduce elaborate chemistry in some cases, we should keep in mind that chemical knowledge will always be needed for a lot of interdisciplinary research projects.

Keywords: AMS

  • Lecture (others)
    VERA-Seminar, Institut für Isotopenphysik, Universität Wien, 28.03.2019, Wien, Österreich

Publ.-Id: 29013

Li-containing liquid metal alloy ion sources for focused-ion beam instrumentation

Mazarov, P.; Nadzeyka, A.; Richter, T.; Yu, Y.; Sanabia, J. E.; Bischoff, L.; Hlawacek, G.; Pilz, W.; Klingner, N.

Focused Ion Beams (FIB) gain an increasing interest in the field of nanotechnology particular for prototyping of microelectronic devices, patterning of 2D materials, high resolution imaging or high resolution ion lithography1. Concerning ion beam resolution and minimization of unwanted damage, light ions like He or Li are preferred candidates. Liquid metal alloy ion sources (LMAIS) with a life time of more than 1000 µAh on the basis of Ga35Bi60Li5 and Sn95Li5 alloys were developed, characterized and finally applied in a commercial mass-separated VELION FIB-SEM system (Raith GmbH). The resolution for imaging and also for the formation of nanostructures using a thin gold film was determined.
In the case of Li ions from the mass separated FIB a lateral resolution of 5.6 nm could be obtained in first experiments2 and the sputter yield was determined to 0.4 for 35 keV Li ions on Au. For reference, the helium ion microscope (HIM) has a lateral resolution of about 0.5 nm and 1.8 nm, for He and Ne respectively, He has a sputter yield of 0.13. For sub-10 nm focused ion beam nanofabrication and microscopy, the GaBiLi-FIB or the SnLi-FIB could therefore be considered alternatives to the HIM with the benefit of providing additional ion species in a mass separated FIB without changing the ion source.

1 L. Bischoff et al. Appl. Phys. Rev. 3, 021 101 (2016).
2 W. Pilz et al. J. Vac. Sci. Technol. B A-18-399 (submitted, 2018).
3 G. Hlawacek et al. J. Vac. Sci. Technol. B 32, 020 801 (2014).

  • Lecture (Conference)
    The 63rd International Conference On ELECTRON, ION, AND PHOTON BEAM TECHNOLOGY AND NANOFABRICATION, 28.-31.05.2019, Minneapolis, United States of America

Publ.-Id: 29012

SiCxNy:Fe films as a tunable ferromagnetic material with tailored conductivity

Pushkarev, R.; Fainer, N.; Kirienko, V.; Matsynin, A.; Nadolinnyy, V.; Merenkov, I.; Trubina, S.; Ehrenburg, S.; Kvashnina, K.

Amorphous ferromagnetic materials with the variable composition are promising candidates for application in rapidlygrowing technological fields, such as spintronics. However, the significant downside of current state-of-art materials is a conductivity mismatch between injector and semiconductor which often is associated with the unavailability to control and precisely tailor magnetic properties and conductivity. We report on the synthesis of soft-magnetic SiCxNy:Fe films with the saturation magnetization of 20 e.m.u./cm3 and conductivity similar to the one of Si, which is crucial for possible applications.
XRD with synchrotron radiation and EXAFS revealed the complex composite structure of the films: crystals of Fe3Si, Fe5Si3, SiC and graphite are embedded into the amorphous matrix of SiCxNy. The variation of deposition conditions allowed us to separately control the magnetic properties through the iron concentration and the conductivity of the material through the amorphous SiCxNy matrix composition. The reported results revealed a significant potential of SiCxNy:Fe films as a prospective object for analysis of spin-polarized transport in amorphous semiconductors and for application in field of spintronics.


Publ.-Id: 29011

Bridging the Green Gap: Metal–Organic Framework Heteromultilayers Assembled from Porphyrinic Linkers Identified by Using Computational Screening

Haldar, R.; Batra, K.; Marschner, S. M.; Kuc, A. B.; Zahn, S.; Fischer, R. A.; Bräse, S.; Heine, T.; Wöll, C.

In organic photovoltaics, porphyrins (PPs) are among the most promising compounds owing to their large absorption cross section, wide spectral range, and stability. Nevertheless, a precise adjustment of absorption band positions to reach a full coverage of the so-called green gap has not been achieved yet. We demonstrate that a tuning of the PP Q- and the Soret bands can be done using a computational approach where substitution patterns are optimized in silico. The Most promising candidate structures were then synthesized. The experimental UV/Vis data for the solvated compounds were in excellent agreement with the theoretical predictions. By attaching further functionalities, which allow using the PP chromophores as linkers for the assembly of metal-organic frameworks (MOFs), we were additionally able to exploit packing effects resulting in pronounced red shifts, which allowed to further optimizing the photophysical properties of PP assemblies. Finally, we use a layer-by-layer method to assemble the PP linkers into surface-mounted MOFs (SURMOFs), thus obtaining high optical quality, homogeneous and crystalline multilayer films. Experimental results are in full accord with the calculations, demonstrating a huge potential of computational screening methods in the tailoring of MOF and SURMOF photophysical properties.


Publ.-Id: 29010

Synthesis and Functionalization of Radium-doped Barium Sulfate Nanoparticles

Reissig, F.; Bauer, D.; Pietzsch, H.-J.; Steinbach, J.; Mamat, C.

The radionuclides radium-223 and radium-224 are two alpha-emitting radionuclides with suitable properties for the TAT. To this date, radium-223 in form of [223Ra]radium chloride (Xofigo) is the only EMA and FDA approved alpha-emitting radiopharmaceutical. Due to its calcimimetic behavior, the radium ion is a bone-seeking therapeutic. To extend the radiopharmaceutical potential of both radionuclides, novel carrier systems have to be developed. Therefore, it is appropriate to investigate different kinds of nanoparticles for their ability to transport radium. Especially, a barium sulfate matrix seems to be sufficient since the principle of co-precipitating the sulfates of radium and barium allows an easy and fast synthesis of radium-doped nanoparticles. Beyond the incorporation of alpha-emitting radionuclides like radium-223 and radium-224, the homologue radionuclide barium-131 can be incorporated as well. Barium 131 decays by electron capture and provides suitable properties for diagnostic applications in nuclear medicine. Radium-223/-224 and barium-131 form a matched pair for new theragnostic approaches. In our research group, we are developing simple methods for the synthesis of small radiolabeled radium/barium sulfate nanoparticles. Furthermore, we are investigating suitable surface functionalizations to attach biological targeting moieties.

Keywords: Bariumsulfat; Radium-224; Nanopartikel

  • Poster
    11th International Symposium on Targeted-Alpha-Therapy, 01.-06.04.2019, Ottawa, Kanada
  • Open Access Logo Abstract in refereed journal
    Journal of Medical Imaging and Radiation Sciences 50(2019)1, S38-S38
    DOI: 10.1016/j.jmir.2019.03.117

Publ.-Id: 29009

Synthese neuartiger Calix[4]arenkäfige für die stabile Bindung von Ba2+ und Ra2+

Mamat, C.; Reissig, F.; Steinbach, J.; Pietzsch, H.-J.

Therapieansätze in der Nuklearmedizin mit Radium-223 beschränken sich zurzeit auf die Behandlung von Knochenmetastasen. Ziel ist es, das Anwendungsfeld für Radium-223 zu erweitern. Dafür werden Liganden entwickelt, die Radium-223 stabil binden und gleichzeitig eine spezifische Erkennungssequenz für diverse Krebsentitäten besitzen. Calixkronen mit funktionalisierten Seitenketten sind dafür vielversprechend.

Calix[4]krone-6-derivate mit Trifluormethylsulfonyl- [1] und 4-Nitrophenylsulfonyl-Seitenketten wurden synthetisiert und mittels NMR und UV/Vis auf ihre Komplexierungseigenschaften für Ba2+ untersucht. Anschließend wurden mittels eines Extraktionsassays Komplexierungen durchgeführt und die resultierenden Komplexe auf ihre Stabilität in Gegenwart anderer Ionen wie Ca2+ untersucht. Die Extraktionsversuche wurden im Chloroform/Wasser-Zweiphasensystem durchgeführt. Dabei wurde eine wässrige Metallsalzlösung ([133Ba]Ba2+ c.a. bzw. [224Ra]Ra2+ n.c.a.) definierter Konzentration vorgelegt und mit einer definierten Stoffmenge des jeweiligen Liganden in Chloroform für 1 h bei RT extrahiert.
Die beiden Calixarenderivate wurden in einer vierstufigen Synthese hergestellt. Anschließende Komplexierungsversuche mit Ba(ClO4)2 verliefen erfolgreich und die Komplexe wurden mittels NMR-Spektroskopie nachgewiesen. Für beide Liganden wurden Stabilitätskonstanten von 5,3-6,3 (Ba2+) bzw. 5,8 (Ra2+) berechnet. Die Radiumkomplexe beider Liganden waren gegenüber Ca2+-Ionen stabil (Release <5%), der Bariumkomplex des Nitrophenylsulfonylliganden war ebenfalls stabil (Release <5%), der des Trifluormethylsulfonylliganden zeigte 30% Release.
Die Wahl der sterisch anspruchsvollen und elektronenziehenden Sulfonylgruppen hatte positive Auswirkungen sowohl auf das Komplexierungsverhalten mit Ba2+ und Ra2+ als auch auf die Stabilität der resultierenden Komplexe in Gegenwart von zweiwertigen Fremdionen.

Keywords: Barium-133; Radium-224; Calixaren

  • Lecture (Conference)
    57. Jahrestagung der DGN 2019, 03.-06.04.2019, Bremen, Deutschland
  • Abstract in refereed journal
    Nuklearmedizin 58(2019), 136
    DOI: 10.1055/s-0039-1683562


  • Secondary publication expected

Publ.-Id: 29008

Synthesis and Biological Investigation of A Novel Fluorine-18 Labeled Benzoimidazotriazine: A Potential Radioligand for In Vivo Phosphodiesterase 2A (PDE2A) PET imaging

Ritawidya, R.; Teodoro, R.; Wenzel, B.; Kranz, M.; Toussaint, M.; Dukic-Stefanovic, S.; Deuther-Conrad, W.; Scheunemann, M.; Brust, P.

Objectives: Cyclic nucleotide phosphodiesterase 2A (PDE2A), an enzyme which hydrolyzes the second messengers cAMP and cGMP, is highly enriched in distinct areas of the brain. Accordingly, PDE2A is involved in important signaling pathways related to normal brain function but also to
neurodegeneration and neuro-oncology [1]. To enable the visualization of this protein in the brainwith PET, we developed a novel fluorine-18 radioligand for PDE2A.
Methods: Based on the benzoimidazotriazine (BIT) tricyclic scaffold, several fluorine-containing derivatives were synthesized via a multi-step synthesis route, and their inhibitory profiles were assessed by PDE isoenzyme-specific activity assays. The most potent and selective PDE2A ligand
BIT1 was radiolabeled via nucleophilic aromatic substitution of the corresponding 2-nitro pyridine precursor by [18F]fluoride in DMSO with thermal heating (Figure 1). [18F]BIT1 was isolated using semi-preparative HPLC (Reprosil-Pur C18-AQ column, 250 x 10 mm, 46% ACN/aqu. 20 mM
NH4OAc, flow 5.5 mL/min) followed by final purification with solid-phase extraction and formulation in isotonic saline containing 10% ethanol. Preliminary in vitro autoradiography and in vivo PET studies (60 min dynamic PET imaging, nanoScan® PET/MRI, MEDISO, Budapest, Hungary) of [18F]BIT1 were performed using pig brain slices and female CD-1 mice, respectively. The in vivo metabolism of [18F]BIT1 was investigated by radio-HPLC analysis of mouse plasma and brain samples at 30 min p.i.
Results: From the series of BIT derivatives, BIT1 was selected as candidate for PET imaging of PDE2A based on the most suitable inhibitory potential and profile (IC50 PDE2A3 = 3.3 nM;16-fold selectivity over PDE10A). [18F]BIT1 was successfully synthesized with a radiochemical yield of 54 ± 2% (n = 3, EOB), molar activities of 155 – 175 GBq/μmol (EOS) and radiochemical purities of ≥99%. [18F]BIT1 was stable in saline, pig plasma, and n-octanol up to 60 min at 37 °C. The distribution pattern of [ 18F]BIT1 in pig brain cryosections corresponds to the spatial distribution of PDE2A with accumulation in the striatal regions caudate nucleus and nucleus accumbens. Additionally, the displacement of [18F]BIT1 with BIT1 as well as TA1 (a potent PDE2A ligand) indicated saturability and selectivity of these binding sites. Uptake of [18F]BIT1 in the brain was shown by subsequent imaging studies in mice (SUVwhole brain = 0.7 at 5 min p.i.); however, more detailed analyses revealed nonspecific distribution of the tracer in the brain (78% parent compound at 30 min p.i.).
Conclusions: The potent and selective PDE2A inhibitor [18F]BIT1 binds in vitro in brain regions known to express PDE2A. Further structural modifications will be performed to develop radiotracers with improved brain uptake and target-selective accumulation in vivo.
1. Deutsche Forschungsgemeinschaft (German Research Foundation, SCHE 1825/3-1).
2. Scholarship Program for Research and Innovation in Science and Technology Project
(RISET-PRO)-Indonesia Ministry of Research, Technology and Higher Education (World
Bank Loan No: 8245-ID)

[1] S. Schröder, B. Wenzel, W. Deuther-Conrad, M. Scheunemann, P. Brust, Novel Radioligands
for Cyclic Nucleotide Phosphodiesterase Imaging with Positron Emission Tomography: An Update
on Developments Since 2012, Molecules 21 (2016) 650–685.

Keywords: Phosphodiesterases; positron emission tomography; molecular imaging; benzoimidazotriazines

  • Poster
    International Symposium in Radiopharmaceutical Sciences, 26.-31.05.2019, Beijing, China

Publ.-Id: 29007

The effect of tumor volume changes on the boost-volume coverage in glioblastoma patients

Hessen, E.; Nijkamp, J.; Troost, E.; Makocki, S.; de Jong, M.; Dewit, L. H. G.; Jasperse, B.; van der Heide, U.; Borst, G.

Purpose/Objective: Radiotherapy is one of the main treatment modalities in the multimodal therapy of glioblastoma patients. The ongoing NRG-BN001 trial (NCT02179086) is evaluating whether boosting a sub-volume with photons or protons improves overall survival as compared to standard-dose photon irradiation. We hypothesize that anatomical changes during irradiation may affect the dose coverage and that these changes may have a greater impact on proton treatment plans compared to photon treatment plans.
Material & Methods: For 24 glioblastoma patients, the MRI was repeated half way during radiation treatment. Three patients had a gross total resection (GTR), four patients underwent a biopsy and 17 patients had a subtotal resection (STR). These patients were treated according to the EORTC-ACROP guideline. A simulated photon and proton treatment plan (intensity modulated proton therapy; IMPT) according to the NRG-BN001 trial were made retrospectively. In this trial, patients in the experimental arm receive a dose of 46Gy/30fr on the T2w/FLAIR abnormalities and 75Gy/30fr on the planning target boost volume (PTV-7500). The PTV-7500 was defined as the resection cavity and/or contrast enhancing lesion on the T1w post gadolinium sequence of the MRI plus a margin of 5 mm (CTV) plus a 4 mm expansion in all dimensions. The trial constraints states that at least 95% of the PTV-7500 should receive 75Gy. To analyze the effect of anatomical changes during treatment on the dose coverage, we evaluated the planned dose distribution (based on the planning MRI) on the delineated PTV-7500 of the repeated MRI.
Results: The median time interval between the two MRIs was 25.5 days (range 15 – 36 days). Between the two scans, the PTV-7500 volume changed with a median of -0.1cc. However, we observed a wide range of -52.8 to +52.2cc. For the photon treatment plans we observed that 83% (n=20) of the patients showed a decline in PTV-7500 coverage (corresponding with a median decline of 6.5% and 8.3cc). The quartile of patients (n=6) with the largest PTV-7500 increase showed a 10% reduction in dose coverage (corresponding with a median volume of 33.2cc). There was no significant difference in coverage changes of the boost volume between the GTR, biopsy only and STR patients (p=0.632). The evaluation of the IMPT plans is ongoing and will be presented during the conference.
Conclusion: During fractionated radiation treatment for glioblastoma patients we observed large target volumetric changes in the boost volume half way during treatment. These target volume changes may lead to substantial declines in dose coverage when patients are treated according to dose-escalation protocol boosting specific sub-volumes. Thus, an important subset of glioblastoma patients may benefit from an MRI guided dose escalation strategy.

  • Lecture (Conference)
    ASTRO, 15.-18.09.2019, Chicago, USA
  • Open Access Logo Abstract in refereed journal
    International Journal of Radiation Oncology Biology Physics 105(2019)1, E99-E100
    DOI: 10.1016/j.ijrobp.2019.06.2290

Publ.-Id: 29006

Robust optimization of dose-volume metrics for prostate HDR-brachytherapy incorporating target and oar volume delineation uncertainties

Balvert, M.; Den Hertog, D.; Hoffmann, A. L.

In radiation therapy planning, uncertainties in the definition of the target volume yield a risk of underdosing the tumor. The traditional corrective action in the context of external beam radiotherapy (EBRT) expands the clinical target volume (CTV) with an isotropic margin to obtain the planning target volume (PTV). However, the EBRT-based PTV concept is not directly applicable to brachytherapy (BT) since it can lead to undesirable dose escalation. Here, we present a treatment plan optimization model that uses worst-case robust optimization to account for delineation uncertainties in interstitial high-dose-rate BT of the prostate. A scenario-based method was developed that handles uncertainties in index sets. Heuristics were included to reduce the calculation times to acceptable proportions. The approach was extended to account for delineation uncertainties of an organ at risk (OAR) as well. The method was applied on data from prostate cancer patients and evaluated in terms of commonly used dosimetric performance criteria for the CTV and relevant OARs. The robust optimization approach was compared against the classical PTV margin concept and against a scenario-based CTV margin approach. The results show that the scenario-based margin and the robust optimization method are capable of reducing the risk of underdosage to the tumor. As expected, the scenario-based CTV margin approach leads to dose escalation within the target, whereas this can be prevented with the robust model. For cases where rectum sparing was a binding restriction, including uncertainties in rectum delineation in the planning model led to a reduced risk of a rectum overdose, and in some cases, to reduced target coverage.© 2019 INFORMS

Keywords: Brachytherapy; Delineation uncertainties; Mixed-integer linear optimization; Robust optimization; Treatment planning

Publ.-Id: 29005

Solving the Kuramoto Oscillator Model on Random Graphs

Kelling, J.; Ódor, G.; Gemming, G.

The problem of synchronization is recently attracting much attention because it relates to current topics in science. The dynamics of electrical grids can be affected by de-synchronizations between supplier and consumer nodes. In brains, synchronization of neuronal activity plays an important role in most functions. The Kuramoto model describes systems of coupled oscillators which, which exhibit non-trivial behavior on complex graphs, making it a suitable tool to study the synchronization dynamics of brains an other systems.

Numerical solution of Kuramoto type ordinary differential equations for long times and large systems requires strong computation power, due to the inherent chaoticity of this nonlinear system.

This poster presents a GPU implementation of a solver achieving large speedups over CPU on sparse random graphs. The key to performance here, is the presented memory layout which supplements the SIMT usage of our design.

  1. extended abstract
The problem of synchronization is recently attracting much attention because it relates to current topics in science. The dynamics of electrical grids can be affected by de-synchronizations between supplier and consumer nodes. In brains, synchronization of neuronal activity plays an important role in most functions.
Using the Kuramoto model[1], we are studying a range of problems, from basinc questions about synnchronisation transitions on disordered lattices and random graphs to problems mentioned in the short abstract. The model shows komplex behavior on human connectome graph, which allow the study of synchronization in the human brain[2]. An extension of the model allows modeling power grid networks[3,4].
Very intensive Simulations are required to obtain precise result especiall near criticality, which these systems show at synchronization transitons. To enable the study of these systems at sufficent precision, we implemented a GPU code, which we are presenting in this poster. To this end we used boost::odeint to get the standart numerical integartion out of the way an focus on the most performance critical aspect: the evaluation of the model itself. The key to our implementation is the choice of SIMT vectorization and a suitable memory layout, which are presented in the poster. The aspects also remain the same, when we add the extension to the second-order Kuramoto Model[2], which is required to model powergrids.
[1] Kuramoto, Y. In Araki, H. (ed.) Mathematical Problems in Theoretical Physics, vol. 39 of Lecture Notes in Physics, Berlin, 420
[2] Villegas, P., Moretti, P. & Muñoz, M. A. Scientific Reports 4, 5990 (2014).
[3] Filatrella, G., Nielsen, A. H. & Pedersen, N. F. Eur. Phys. J. B 61, 485–491 (2008)
[4] Ódor, G. & Hartmann, B. Phys. Rev. E 98, 022305 (2018).

Keywords: GPGPU; random graph; Kuramoto model

Publ.-Id: 29004

Beneficiation of parisite-rich rare earth ore from the Nam Xe South deposit, Vietnam

Möckel, R.; Heinig, T.; Cardenas Vera, A. F.; Gutzmer, J.; Merker, G.; van Phan Quang, .

Parisite-rich rare earth element (REE) ores from the Nam Xe deposit in northern Vietnam were beneficiated on a lab scale. Beneficiation experiments included, amongst others, sensor-based sorting, magnetic separation and flotation. Particular analytical focus during all experiments was set on the grain size, association and intergrowth of of the main REE carrier mineral parisite, which is finely intergrown with minerals of the barite-celestine solid solution series. All experiments were accompanied by mineral liberation analysis and chemical assays in order to be able to provide direction towards an optimal beneficiation strategy for this REE ore with its rather unique mineralogy. Special focus was set on the grain characteristics of the main REE carrier mineral parisite, which is finely intergrown above all with minerals from the barite-celestine solid solution series.
A multi-stage flotation technique was developed that uses an ambient rougher and a hot cleaner stage. Concentrates with 40% TREO grade with a total recovery of about 80% were achieved. It was shown that a combination with a sensor-based pre-sorting prior to the flotation can increase the input grade for flotation considerably by a nearly loss-free rejecting of virtually barren bed rock. The process combination developed holds good potential for further improvements.

  • Lecture (Conference)
    15th Biennial Meeting of the Society for Geology Applied to Mineral Deposits, 27.-30.08.2019, Glasgow, Scotland

Publ.-Id: 29003

Fragment molecular orbital (FMO) method for studying actinide/lanthanide interaction with DNA/protein

Tsushima, S.; Mochizuki, Y.; Fahmy, K.

Due to its potential health and environmental impacts, actinide binding to biomolecules has been a subject of intensive investigations. A large number of experimental works have been carried out but our understanding remains mostly in a macroscopic scale. Modeling actinide interaction with large biomolecules using ab initio quantum chemical calculations may drastically expand our molecular level knowledge but is challenged by a demand for huge computational resources.
Our strategy to overcome this difficulty is to apply fragment molecular orbital (FMO) method. In FMO, the molecular system of interest is partitioned into small fragments. Each fragment and fragment pair is subject to self-consistent field calculations under environmental electrostatic potentials and the electronic structure of the whole system is reconstituted [1]. This procedure drastically reduces computational cost of Hartree Fock calculations from N3 to N2 (or less) and is readily parallelizable. FMO has been extended to MP2 and to DFT to include electron correlation and was successfully applied to the systems such as hydrated DNA [2].
Currently we are upgrading the FMO program Abinit-MP [3] to implement 5f elements into the program. We first choose uranyl-bound DNA for a case study. Calculations are performed as follows. UO22+-bound d(CGCGAATTCGCG)2 (Dickerson-Drew dodecamer) with 20 Na+ ions and SPC/E water shell with 10 Å thickness is first thermally equilibrated and subsequently submitted to MD simulation at 300 K for 100 ns interval using AMBER 14 program. Force field parameters for UO22+ and coordinating water are those developed by Pomogaev et al. [4]. At each 1 ns time step of MD simulation, the structure is extracted and submitted to FMO single point energy calculation at the MP2 level. In FMO, nucleic unit is appropriately divided into sugar, base, and phosphate fragments. Inter-fragment interaction energy analysis is performed to explore the binding affinity of uranyl to DNA and its influence on base pairing.
[1] K.Kitaura et al. (1999) Chem. Phys. Lett. 313, 701–706.
[2] K.Fukuzawa et al. (2015) Comput.Theor.Chem. 1054, 29–37.
[3] S.Tanaka et al. (2014) Phys. Chem. Chem. Phys. 16, 10310–10344.
[4] V.Pomogaev et al. (2013) Phys. Chem. Chem. Phys. 15, 15954–15963.

  • Poster
    Joint 12th EBSA and 10th ICBP-IUPAP Biophysics Congress, 20.-24.07.2019, Madrid, Spain

Publ.-Id: 29002

Observations of Coherent Optical Transition Radiation Interference Fringes Generated by Laser Plasma Accelerator Electron Beamlets

Lumpkin, A.; Laberge, M.; Rule, D.; Zgadzaj, R.; Hannasch, A.; Downer, M.; Zarini, O.; Bowers, B.; Irman, A.; Couperus, J.; Debus, A.; Kohler, A.; Schramm, U.

We report initial observations of coherent optical transition radiation interferometry (COTRI) patterns generated by microbunched electrons from laser-driven plasma accelerators (LPAs). These are revealed in the angular distribution patterns obtained by a CCD camera with the optics focused at infinity, or the far-field, viewing a Wartski two-foil interferometer. The beam divergences deduced by comparison to results from an analytical model are sub-mrad, and they are smaller than the ensemble vertical beam divergences measured at the downstream screen of the electron spectrometer. The transverse sizes of the beamlet images were obtained with focus at the object, or near field, and were in the few-micron regime as reported by LaBerge et al. [8]. The enhancements in intensity are significant relative to incoherent optical transition radiation (OTR) enabling multiple cameras to view each shot. We present two-foil interferometry effects coherently enhanced in both the 100-TW LPA at 215 MeV energy at Helmholtz-Zentrum Dresden-Rossendorf and the PW LPA at 1.0-GeV energy at the University of Texas-Austin. A transverse emittance estimate is reported for a microbunched beamlet example generated within the plasma bubble.

Keywords: LPA; microbunching; COTR; beam size; divergence

  • Contribution to proceedings
    18th Advanced Accelerator Concepts Workshop (AAC 2018), 12.-17.08.2018, Breckenridge, CO, USA
    2018 IEEE Advanced Accelerator Concepts Workshop (AAC): IEEE, 978-1-5386-7721-6
    DOI: 10.1109/AAC.2018.8659381

Publ.-Id: 29001

Bacillus safensis JG-B5T affects the fate of selenium by extracellular production of colloidally less stable nanoparticles

Fischer, S.; Krause, T.; Lederer, F.; Merroun, M. L.; Shevchenko, A.; Hübner, R.; Stumpf, T.; Jordan, N.; Jain, R.

Bacteria strain Bacillus safensis JG-B5T is an obligate aerobic microorganism isolated from uranium mining waste pile. The role played by this microorganism in the transport of selenium is poorly understood. This study demonstrated that B. safensis JG-B5T can reduce 70 % of 2.5 mM selenite whereas selenate reduction was not observed. Formation of the resulting biogenic elemental selenium nanoparticles (BioSeNPs) occurred exclusively extracellularly. The ζ-potential of the produced BioSeNPs varied from −44.2 (±0.2) mV to −10.6 (±3.3) mV when Na+:Se ratio was varied from 0 to 0.8 (mM:mM), suggesting a lower colloidal stability. Further experiments in two-chamber reactors and transmission electron microscopy revealed that direct cell contact is essential for selenite reduction by B. safensis JG-B5T. The selenite reduction is likely primarily mediated through membrane-associated proteins, like succinate dehydrogenase as revealed by genome and proteomics analysis. Altogether, this study showed that aerobic bacteria B. safensis JG-B5T is involved in decreasing the environmental bioavailability and toxicity of selenium by membrane protein-mediated reduction of selenite oxyanions and formation of extracellular BioSeNPs with low colloidal stability.

Keywords: Obligate aerobic; two-chamber reactor; proteomics; membrane-associated proteins; selenite

Publ.-Id: 29000

Photocatalytic Oxygenation of Cyclohexene Initiated by Excitation of [UO2(OPCyPh2)4]2+ under Visible Light

Mashita, T.; Tsushima, S.; Takao, K.

Oxygenation reaction of cyclohexene was studied under presence of a 4-fold UO22+ complex with cyclohexyldiphenylphosphine oxide, [UO2(OPCyPh2)4]2+, and blue light irradiation at 436 nm in acetonitrile. As a result, 1,6-hexanedial, cyclohexene oxide, 2-cyclohexen-1-one, and 2-cyclohexen-1-ol were photocatalytically generated as oxygenated products with TOF = 6.7 h−1. In contrast, dimerization of cyclohexene was observed under Ar atmosphere. This implies that a hydrogen atom at the allyl position is abstracted by photoexcited *[UO2(OPCyPh2)4]2+ to give a cyclohexene radical and a U(V) intermediate [UVO2(OPCyPh3)4]+, being well supported by DFT calculation. Under O2 atmosphere, the former reacts with dissolved O2 to give 2-cyclohexen-1-one and 2-cyclohexen-1-ol. Dissolved O2 would be activated by the U(V) intermediate to afford O22− in the end, which drives oxygenation of C=C bond of unreacted cyclohexene.

Publ.-Id: 28999

Sensitivity and uncertainty analysis for geochemical models for repository safety assessment

Stockmann, M.; Becker, D.-A.; Noseck, U.; Brendler, V.

A key component of safety assessment for radioactive waste repositories in deep geological formations is the simulation of potential radionuclide release scenarios and the transport of radionuclides through the repository system. The realistic modelling of (hydro-)geochemical processes is of high relevance for assessing the migration of radionuclides in groundwater systems. One important retardation process for radionuclides to be considered is sorption onto mineral surfaces of the host rock / sediments. Due to the heterogeneities of the natural system and the high complexity of the geochemical models with uncertain or varying input parameters, it is important to understand which of the input parameter uncertainties have considerable influences on the model output uncertainty. This in turn allows model reduction required to upscale from the molecular to the plug scale. Consequently, we performed sensitivity and uncertainty analysis (SA/UA) to investigate and understand our geochemical model.
For the quantification of the contaminant retention in groundwater, the solid/liquid distribution coefficients (Kd-values) calculated for a given groundwater/rock system are traditionally used. Most often conventional concepts with constant Kd values are applied in reactive transport simulations. Such an approach has the advantage to be simple and computationally fast but cannot reflect changes in geochemical conditions that will occur during the evolution of the repository system, e.g. due to climatic changes. Due to the German safety criteria with an assessment period of about 1 million years it is necessary to consider the impact of such geochemical changes on the radionuclide transport and retardation. For this, we developed a new approach, where the smart Kd concept ( [1] is modified in complex geochemical models including mechanistic sorption models, and implemented it in reactive transport calculations [2, 3]. Possible migration scenarios for repository-relevant radionuclides (isotopes of Am, Cm, Cs, Ni, Np, Pu, Ra, Se, Th and U) through a typical sedimentary rock system covering potential repository host rocks, namely salt and clay formations in Northern Germany as natural geological barrier, were developed in the first stage.
Smart Kd-values and their associated sensitivities and uncertainties were computed for a wide range of important geochemical input parameters / boundary conditions such as pH value, ionic strength, concentration of competing cations and complexing ligands, e.g. dissolved inorganic carbon (DIC) and calcium (Ca2+). Our toolbox coupled the geochemical speciation code PHREEQC [4] with the numeric tool UCODE [5] and SimLab2.2/4 [6]. SimLab has the advantage to permit a simultaneous variation of all input parameters according to their probability density functions and mutual correlations. It provides (in contrast to UCODE, which also incorporates some simple SA/UA algorithms) methods for Global SA. Comparable SA/UA have been done with a new software package RepoSUN, which is based on SimLab4 [7]. For the varying parameters uncertainty intervals were defined from field investigations and log-uniform distributions were assumed for all parameters, except for the pH value, which was assumed to be uniformly distributed. The results, i. e. the smart Kd values, were analyzed in the following way:
o As the output distribution covers several orders of magnitude, a log-transformation was performed on the output data. Then the computed a-priory multidimensional smart Kd matrices (see for U(VI) in Fig. 1, left) are accessible for interpolations during subsequent transport simulations.
o A histogram of the model output visualizes the distribution (see for U(VI) in Fig. 1, right).
o Some statistical measures were calculated to characterize the distribution (minimum, maximum, mean, standard deviation).
o Sensitivity measures were calculated for each of the input parameters: the standardized regression coefficient (SRC), the standardized rank regression coefficient (SRRC) and the variance-based first-order sensitivity index (SI1).
On the basis of the results it could be shown that the smart Kd approach goes considerably beyond the conventional concepts. We could illustrate that constant Kd values (see for U(VI) in Fig. 1, right, green line) used in previous transport simulations [8] are a crude assumption, as in reality they rather range over several orders of magnitude. Moreover, with the results from the SA, the most important input parameters influencing the radionuclide retardation can be identified (key parameters of the model). The calculated sensitivity indices allowed us to assess the most and less sensitive parameters. From the visualized smart Kd matrix for U(VI) (Fig. 1, left) it is obvious that mainly the pH value and the DIC influences the sorption of U(VI) under the given conditions. SA is a useful means for reducing the complexity of a geochemical model by focusing on the most important input parameters.

  • Poster
    Ninth International Conference on Sensitivity Analysis of Model Output (SAMO'19), 28.-30.10.2019, Barcelona, Spain

Publ.-Id: 28998

Time efficient scatter correction for time-of-flight PET: the immediate scatter approximation

Nikulin, P.; Maus, J.; Hofheinz, F.; Lougovski, A.; van den Hoff, J.

Utilization of Time-Of-Flight (TOF) information allows to improve image quality and convergence rate in iterative PET image reconstruction. In order to obtain quantitatively correct images accurate scatter correction (SC) is required that accounts for the non-uniform distribution of scatter events over the TOF bins. However, existing simplified TOF-SC algorithms frequently exhibit limited accuracy while the currently accepted gold standard — the TOF extension of the single scatter simulation approach (TOF-SSS) — is computationally demanding and can substantially slow down the reconstruction. In this paper we propose and evaluate a new accelerated TOF-SC algorithm in order to improve this situation. The key idea of the algorithm is the use of an immediate scatter approximation (ISA) for scatter time distribution calculation which speeds up estimation of the required TOF scatter by a factor of up to five in comparison to TOF-SSS. The proposed approach was evaluated in dedicated phantom measurements providing challenging high activity contrast conditions as well as in representative clinical patient data sets. Our results show that ISA is a viable alternative to TOF-SSS. The reconstructed images are in excellent quantitative agreement with those obtained with TOF-SSS while overall reconstruction time can be reduced by a factor of two in whole-body studies, even when using a listmode reconstruction not optimized for speed.

Keywords: PET; Scatter Correction; Immediate Scatter Approximation; Image Reconstruction; TOF; SSS; TOF-SSS; TOF-SC; ISA


Publ.-Id: 28997

Towards best practice guidelines for Euler-Euler simulations of poly-disperse bubbly flows

Lucas, D.; Liao, Y.; Rzehak, R.; Krepper, E.

Poly-disperse bubbly flows are involved in normal operation as well as in accident scenarios of Light Water Reactors. There are many activities to qualify CFD-methods for the simulation of safety-relevant processes. However, due to the complexity of such flows many details have to be carefully considered to define a proper setup for such simulations. The present paper aims at the establishment of a guideline how to prepare and conduct such a simulation as well as to evaluate the simulation results according to the best practice. The procedure has to start with an analysis of the expected flow situation, flow parameters and observed phenomena. Accordingly a classification should be done. Beside boundary conditions, the numerical grid, the time stepping and other issues a careful selection of the modelling framework (e.g. inclusion of a population balance, two- or multi-field approach) and the closure models has to be done based on the previous analysis. A set of well suited closure models is defined by the so-called baseline model for poly-disperse flows. Numerical convergence has to be checked throughout the simulation. For the comparison with experimental data possible uncertainties of the input data used and the experimental data used for comparison have to be considered. Besides the presentation of the state of the art best practice guidelines also their limitation and requirements for future research are discussed.

Keywords: CFD; bubbly flow; Euler-Euler; best practice guidelines

  • Contribution to proceedings
    The 18th International Topical Meeting on Nuclear Reactor Thermal Hydraulics (NURETH-18), 18.-22.08.2019, Portland, OR, USA
  • Lecture (Conference)
    The 18th International Topical Meeting on Nuclear Reactor Thermal Hydraulics (NURETH-18), 18.-22.08.2019, Portland, OR, USA

Publ.-Id: 28996

Influence of the bubble size distribution on the bubble column flow regime

Lucas, D.; Ziegenhein, T.

The role of the bubble size dependent lateral lift force on the flow regime is experimentally investigated in a tall bubble column. In the experiments, only the initial bubble size distribution was modified by using a gas sparger with different injection needles and varying the flow through specific injection needles. The gas flow rate was kept unchanged in all experiments. Depending on the bubble size distribution homogeneous, transitional or heterogeneous flow regimes were observed. The flow regime is in good agreement with the predictions from the stability criterion obtained by a previously done linear stability analysis for poly-dispersed flow. It was found that as a rule of thumb the following criterion can be used.
If most of the gas volume is transported by bubbles smaller than the critical diameter at which the lift force changes its sign, the flow is stabilized leading to a homogeneous flow regime. If most of the gas volume is transported by bubbles larger than that diameter the flow is de-stabilized leading a heterogeneous flow regime. If the fraction of gas transported by small and large bubbles is about the same, the initial conditions remain dominant throughout the column height.

Keywords: bubble size; lift force; stability; bubble column; flow regime; regime transition


Publ.-Id: 28995

Separation of transition metal oxoanions from complex feed solutions by solvent extraction

O'Toole, N.; Mansel, A.; Kelly, N.; Scharf, C.

Certain metals, which can be defined as “strategic” due to a predicted high future demand and/or unstable supply, can currently be found trapped in the slag by-products of European steel production.[1-3] Notably these metals include chromium and vanadium. The H2020 project CHROMIC seeks to develop a process for the separation and purification of these metals from the slag matrix host, leaving the slag as a valorisable product for use in e.g. construction. This process will involve selective high-alkaline oxidative leaching of the metal value, followed by solvent extraction (SX) on the alkaline leach solutions thus-produced.
The alkaline and oxidising conditions mean the target metals are present in the form of oxoanions in the leach liquor; therefore a cationic extraction agent, namely Aliquat 336, is employed for the SX method. This extractant has proven capable of selectively removing chromium(VI) and vanadium(V) from complex mixtures representative of leach solutions from industrial slags, with a strong influence of the pH value and the presence of competing anions. To optimise the procedure we use the radiotracer technique, labelling the metal concentration with the produced-in-house isotopes ⁵¹Cr and ⁴⁸V respectively.[4,5] This technique offers many advantages over conventional options, including high precision measurement at extremely low concentrations, no effect of the solvent medium, and no need to further workup the solution after phase separation. Our results indicate that chromium(VI), which is the major species in the leachate feed, is preferentially extracted by the Aliquat 336 system over all other species present under most conditions. Studies are underway to examine the behaviour of Cr(III) in these systems, as this ion may be present in place of Cr(VI).
[1] Report by Grand View Research, Chromium Market Outlook Report By Application (Metallurgy, Chemicals, Refractory), By Region (North America, Europe, Asia Pacific, Central & South America, Middle East & Africa), And Segment Forecasts, 2018 – 2025, Report ID GVR-2-68038-305-8, (2018).
[3] Bio Intelligence Service, Study on data for a raw material system analysis: Roadmap and test of the fully operational MSA for raw materials – Final report, for the EC DG GROW, (2015).
[4] Katsuta et al, Journal of Radioanalytical and Nuclear Chemistry, 222(1-2), 45-50, (1997).
[5] Bonardi et al, Journal of Radioanalytical and Nuclear Chemistry, 263(1), 23-28, (2005).

Keywords: Circular economy; solvent extraction; chromium; vanadium; slag

  • Poster
    Jahrestreffen der ProcessNet-Fachgruppen Phytoextrakte und Extraktion, 07.-08.02.2019, Muttenz, Schweiz

Publ.-Id: 28994

Quantum Critical Dynamics of a Heisenberg-Ising Chain in a Longitudinal Field: Many-Body Strings versus Fractional Excitations

Wang, Z.; Schmidt, M.; Loidl, A.; Wu, J.; Zou, H.; Yang, W.; Dong, C.; Kohama, Y.; Kindo, K.; Gorbunov, D. I.; Niesen, S.; Breunig, O.; Engelmayer, J.; Lorenz, T.

We report a high-resolution terahertz spectroscopic study of quantum spin dynamics in the antiferromagnetic Heisenberg-Ising spin-chain compound BaCo2V2O8 as a function of temperature and longitudinal magnetic field. Confined spinon excitations are observed in an antiferromagnetic phase below TN ≃ 5.5 K. In a field-induced gapless phase above Bc = 3.8 T, we identify many-body string excitations as well as low-energy fractional psinon/antipsinon excitations by comparing to Bethe-Ansatz calculations. In the vicinity of Bc, the high-energy string excitations are found to be dynamically dominant over the fractional excitations.

Publ.-Id: 28993

Protecting Pulsed High-Power Lasers with Real-Time Object Detection

Kelling, J.; Gebhardt, R.; Helbig, U.; Bock, S.; Schramm, U.; Juckeland, G.

In Petawatt laser systems, firing at 10Hz, suddenly appearing scatterers can damage components. Damage(-spreading) can be avoided by suspending operation immediately on occurrence of such an event. This poster presents our approach for the automatic detection of critical failure states in real-time, employing state-of-the-art object localization on intensity profiles of the laser beam.

Learn, how we fitted the You Look Only Once (YOLO) approach, which is suited to low-latency object detection, to our problem and how we adapted the required multi-step training protocol to the available experimental data.
In this application accuracy trumps high recall, as false positives would severely impede productivity or even render our system useless. This had us refrain from general anomaly detection and thus we also present different ways in which we tune the object-detection for minimal false-positive rates.

  1. extended abstract
High-power lasers are operated at our research center for investigations of exotic states of matter and medical applications, among others. This project to improve the automatic shutdown/interlock system of two lasers (one in operation, one currently under construction) has the goal of reducing the probability of, potentially expensive, damage-spreading scenarios, while at the same time avoiding false alarms. In order to achieve high precision, we train for high recall only for known indicators, instead of using anomaly detection.
After we presented a proof-of-concept for this type of failure-state-detection at GTC 2018, where the main challenge was in dealing with a far too small dataset, we are now working on a pure deep-learning approach driven by systematic experimental data. In the new design, intended for production use, the classification takes place on differences between a running average of non-signaling images and the current shot. This is required, because no images can be obtained which can be classified as "good" without context. In order to achieve fast object-detection, to highlight potential problems for the operator, the you look only once (YOLO) approach[1], which we modify by removing the final layers for bounding-box prediction and train the network to directly produce an expressive feature map (lazy YOLO).
From this talk, the audience can learn how we adapted the well-known YOLO approach to our real-world application, from the employed network to the multi-step training protocol. Another topic is the design for short response times, to which end we employ Caffe, OpenCV on GPU and use C++ as main programming language instead of python.
[1] Redmon, J., Farhadi, A.: YOLO9000: Better, Faster, Stronger, ArXiv e-prints, 2016

Keywords: Image Classification; Caffe; automatic Laser-safety shutdown; Object Detection

Publ.-Id: 28992

Dimeric Uranium(VI)–Citrate Complexes: Structures and Dynamics

Kretzschmar, J.; Tsushima, S.; Jäckel, E.; Meyer, R.; Steudtner, R.; Müller, K.; Schmeide, K.; Brendler, V.; Stumpf, T.

The aqueous chemistry of the uranium(VI)–citrate system is challenging, as evidenced by still controversial discussions on complex stoichiometries and structures [1–4]. For a sound understanding of the chemical behavior in general and the environmental fate in particular, knowledge of both aqueous speciation and molecular structures in solution is crucial. Here, complexes formed by the uranyl ion, U(VI), and citrate (Cit) were examined in the pH range 2–8 by combining one- and two-dimensional NMR with UV-Vis, ATR FT-IR, and EXAFS spectroscopies as well as DFT-based quantum chemical calculations.
Upon complexation, a chiral center is induced in Cit’s central carbon, resulting in the formation of two diastereomeric pairs of enantiomers, whereupon the dimeric complexes exhibit syn and anti configured isomers. In fact, the combination of 17O NMR (note: at natural abundance) and DFT calculations allowed an unambiguous decision on complex geometry and overall configurations. It is evidenced for the first time that the syn isomer is favored in aqueous solution in contrast to the preferably crystallizing anti isomer. Both isomers coexist and interconvert among one another, with a rate estimated to be in the order of 10² s¹ at 25 °C in acidic media, and a corresponding activation energy of approximately 60 kJ mol¹.
Upon increasing pH, the ternary dimeric U(VI)–Cit mono- and bis-hydroxo (2:2:1 and 2:2:2) complexes form as evidenced by both UV-Vis and ATR FT-IR spectroscopy. The latter methods provided stability constants (log β): 19.5 (2:2:0), 14.0 (2:2:1), and 6.5 (2:2:2). Accordingly, the process can be referred to as U(VI) hydrolysis within the U(VI)–Cit complex as the two coordinating water molecules in the respective fifth coordination site each abstract H+. Thus, any U(VI)-coordinating water in ever so stable complexes is susceptible to hydrolysis even in strong acidic media as consequence of the interplay between metal ion Lewis acidity and solution pH.
Virtually all single-crystal X-ray structures containing the dimeric U(VI)–Cit complex in any manner, reveal anti configuration, e.g. [4]. The predominance of the syn isomer in solution was hitherto unnoticed, demonstrating that, particularly upon different physico-chemical properties of the isomers, the (crystalline) solid phase does not necessarily reflect speciation and structures found in (aqueous) solution, underlining the importance of rigorous solution studies.

[1] I. Feldman et al., J. Am. Chem. Soc., 1954, 76, 4726.
[2] M. T. Nunes and V. M. S. Gil, Inorg. Chim. Acta, 1987, 129, 283.
[3] S. P. Pasilis and J. E. Pemberton, Inorg. Chem., 2003, 42, 6793.
[4] M. Basile et al., Chem. Commun. 2015, 51, 5306.

Keywords: uranium; uranyl; U(VI); citric acid; molecular structure; NMR; ATR FT-IR; UV-Vis; spectroscopy; ternary complex; uranium hydrolysis; stability constant; isomerization

  • Lecture (Conference)
    Jahrestagung der Fachgruppe Nuklearchemie 2019, 25.-27.09.2019, Dresden, Deutschland

Publ.-Id: 28991

Simultaneous 8.2 keV phase-contrastimaging and 24.6 keV X-ray diffraction fromshock-compressed matter at the LCLS

Seiboth, F.; Fletcher, L. B.; Mcgonegle, D.; Anzellini, S.; Dresselhaus-Cooper, L. E.; Frost, M.; Galtier, E.; Goede, S.; Harmand, M.; Lee, H. J.; Levitan, A. L.; Miyanishi, K.; Nagler, B.; Nam, I.; Ozaki, N.; Rödel, M.; Schropp, A.; Spindloe, C.; Sun, P.; Wark, J. S.; Hastings, J.; Glenzer, S. H.; Mcbride, E. E.

In this work, we demonstrate simultaneous phase-contrast imaging (PCI) and X-ray diffractionfrom shock compressed matter at the Matter in Extreme Conditions endstation, at the LinacCoherent Light Source (LCLS). We utilize the chromaticity from compound refractive X-ray lensesto focus the 24.6 keV 3rd order undulator harmonic of the LCLS to a spot size of 5lm on target toperform X-ray diffraction. Simultaneous PCI from the 8.2 keV fundamental X-ray beam is used tovisualize and measure the transient properties of the shock wave over a 500lm field of view.Furthermore, we demonstrate the ability to extend the reciprocal space measurements by 5 Angstroem, rel-ative to the fundamental X-ray energy, by utilizing X-ray diffraction from the 3rd harmonic of theLCLS.

Keywords: Phase Contrast Imaging; PCI; Matter in Extreme Conditions; MEC; LCLS; shock compression; x-ray diffraction; XFEL; germanium; shock; release


Publ.-Id: 28990

A Polka-Dot Pattern Emerges in Superfluid Helium

Wosnitza, J.

A surprising two-dimensional pattern appears in superfluid helium-3 when the liquid is confined to a micrometer-thick cell and exposed to a magnetic field.

Publ.-Id: 28989

Low anisotropic upper critical fields in SmO1−xFxFeAs thin films with a layered hybrid structure

Haindl, S.; Kampert, E.; Sasase, M.; Hiramatsu, H.; Hosono, H.

We report on the upper critical fields in SmO1−xFxFeAs thin films prepared by pulsed laser deposition. With an F-content gradient along their thickness, the films could be described approximately as layered two-phase hybrid structures comprised of one superconducting layer and one antiferromagnetic layer. An analytical characterization of different thin film samples by Auger electron spectroscopy and energy-dispersive x-ray spectroscopy in scanning transmission electron microscopy is provided and structural defects, such as antiphase boundaries, were confirmed for films grown at lower deposition temperatures. Electrical transport measurements in pulsed magnetic fields yielded upper critical fields higher than 80 T with an anisotropy γHc2 ≤ 2.25.

Publ.-Id: 28988

Microscopic and spectroscopic investigations of the interactions of a Halobacterium-isolate with uranium

Hilpmann, S.; Bader, M.; Bachran, M.; Steudtner, R.; Schmidt, M.; Stumpf, T.; Cherkouk, A.

Rock salt formations are potential host rocks for the long-term storage of high-level radioactive waste in a deep geological repository, besides clay and crystalline rock. There are multiple studies about the geological, geochemical and geophysical properties of these host rocks. However, there exists still a lack of knowledge about indigenous microorganisms and their influence on the chemical speciation. For a long-term risk assessment, it is of high interest to study how these microorganisms interact with radionuclides. Therefore, the interactions of an extremely halophilic archaeon, Halobacterium sp. GP5 1-1 with uranium, one of the major radionuclides of concern, were investigated in detail. This extremely halophilic archaeon was isolated from a German rock salt sample. Different microscopic and spectroscopic methods were combined to decipher the occurring processes on a molecular level.
To investigate the interaction kinetics of uranium(VI) onto the cells of Halobacterium sp. GP5 1-1, time-dependent association experiments with two different uranium(VI) concentrations were performed. At both concentrations the amount of bioassociated uranium(VI) increased with the incubation time. It was determined that the association process at the higher concentration (30 µM) was much slower than the kinetic at the lower uranium(VI) concentration (10 µM).
Various microscopic and spectroscopic methods were used to understand the interaction mechanisms on a molecular level. Overall, the association process is not exclusively a biosorption, which is a passive process and in general completed after a short time of incubation (0 – 2 h) [1]. The microscopic images of the live/dead staining show the formation of cell agglomerates after a certain exposition time at both concentrations. During the process, organic matter is excreted from the cells. Therefore, more functional groups are available for further uranium(VI) binding.
Electron microscopic images of the cells allowed drawing conclusions about different microbe-radionuclide interactions at different uranium(VI) concentrations. A biomineralization takes place at lower concentrations (10 µM) and uranium(VI) is bound to biofilm-like structures at higher concentrations (60 µM).
Using time-resolved laser-induced luminescence spectroscopy, different aqueous species could be extracted from the supernatant. These species differ slightly in dependence on the uranium(VI) concentration. In both cases, a uranyl-carbonate-complex is formed during the association process due to microbial released CO2. Additionally the formation of a phosphate species in the cell pellets at low uranium(VI) concentrations was observed in a uranium(VI) concentration-dependent experiment (10-60 µM). In contrast, at higher uranium(VI) concentrations a carboxylic species was formed. This is in agreement with the already mentioned excretion of organic matter from the cells during the uranium(VI) incubation.
These findings offer new insights into the microbe-actinide interactions at highly saline conditions relevant to high-level radioactive waste disposal in rock salt.[1]

[1] J. R. Lloyd, L. E. Macaskie (2002) in “Interactions of Microorganisms with Radionuclides” (Eds.: M.J. Keith-Roach, F. R. Livens), Elsevier, pp. 313-381

  • Lecture (Conference)
    Migration 2019, 15.-20.09.2019, Kyoto, Japan

Publ.-Id: 28987

Complex formation between UO22+ and α-isosaccharinic acid: insights on a molecular level

Brinkmann, H.; Patzschke, M.; Kaden, P.; Raiwa, M.; Rossberg, A.; Kloditz, R.; Heim, K.; Moll, H.; Stumpf, T.

Cellulosic materials present as tissue, paper, wood, or filter materials in low and intermediate level waste will degrade under alkaline conditions if water ingresses in a cementitious backfilled repository. The main degradation product is isosaccharinic acid. Complex formation with isosaccharinic acid may adversely affect the retention of radionuclides by sorption or formation of solid phases. Hence, this compound is of particular concern in the context of nuclear waste disposal. Structural information of complexes are limited to spherical metal centers and little is known about the interaction of uranyl (UVIO22+) with isosaccharinic acid. Therefore, the interaction of UO22+ with α-isosaccharinate (ISA) was studied under acidic conditions focusing particularly on the structural characterization of the formed complexes. Attenuated total reflection Fourier-transform infrared (ATR-FTIR), nuclear magnetic resonance (NMR), UV-Vis, extended X-ray absorption fine structure (EXAFS) spectroscopy and electrospray-ionization mass spectrometry (ESI-MS) were combined with theoretical calculations to obtain a process understanding on the molecular level. The dominant binding motifs in the formed complexes are 5- and 6-membered rings involving the carboxylic group as well as the α- or β-hydroxy group of ISA. Two concentration dependent complex formation mechanisms were identified involving either mono- ([UO2(ISA)(H2O)3]+) or binuclear ([(UO2)2(ISA)(H2O)6]3+) species. Furthermore, this study unveils the interaction of UO22+ with the protonated α-isosaccharinic acid (HISA) promoting its transformation to the corresponding α-isosaccharinate-1,4-lactone (ISL) and inhibiting the formation of polynuclear UO22+-ISA species. Future studies on related systems will benefit from the comprehensive knowledge concerning the behavior of ISA as complexing agent gained in the present study.

Keywords: Uranium; Isosaccharinic acid; Complexation; Lactonization; Spectroscopy

Publ.-Id: 28986

From Exploration towards Predictive Geometallurgy - The Role of SEM-based Automated Mineralogy and Statistical Assessment

Birtel, S.; Bachmann, K.; Büttner, P.; Tolosana Degado, R.; van den Boogaart, K. G.; Gutzmer, J.

Geometallurgical models are constructed to quantitatively predict how ores will behave during extraction and beneficiation. Depending on data availability, complexity of data and operational stage different classes of geometallurgical models can be distinguished: 1) resource potential, 2) recoverable resources, 3) first order predictive models, 4) predictive models, and 5) real-time mining models. Here, two case studies are presented where modal mineralogy and microstructural data obtained from SEM-based image analysis are combined with complementary analytical data and statistically assessed in order to predict raw material behaviour during mineral processing. For both case studies, the necessary steps to develop existing models into truly predictive geometallurgical models are outlined. The first case study concerns the recovery of Sn from a historic flotation tailings storage facility. The second case study centres on the recovery of PGE as by-products from a chromite ore deposit as a first order predictive geometallurgical model.

Keywords: SEM based automated mineraloy; statistcal assement; case studies; process optimization

  • Contribution to proceedings
    15th Biennial Meeting of the Society for Geology Applied to Mineral Deposits, 27.-30.08.2019, Glasgow, UK
    Proceedings to 15th Biennial Meeting of the Society for Geology Applied to Mineral Deposits, 1474-1477
  • Lecture (Conference)
    15th Biennial Meeting of the Society for Geology Applied to Mineral Deposits, 27.-30.08.2019, Glasgow, UK

Publ.-Id: 28985

Photogeneration of Manganese(III) from Luminescent Manganese(II) Complexes with Thiacalixarene Ligands: Synthesis, Structures and Photophysical Properties

O'Toole, N.; Lecourt, C.; Suffren, Y.; Hauser, A.; Khrouz, L.; Jeanneau, E.; Brioude, A.; Luneau, D.; Desroches, C.

The photophysical properties of the compound [(ThiaSO₂)(MnII)₂(DMF)₄(H₂O)₂] (2), ThiaSO₂ = p-tert-butylsulfonylcalix[4]arene, are presented and compared to the ones of [(ThiaSO₂)₂(MnII)₄F]K (1). The orange luminescence of 2 is attributed, as for 1, to the MnII centred ⁴T₁→⁶A₁ transition and shows, for this type of complex, the weak influence of the Mn²⁺ coordination and ThiaSO₂ conformation on this luminescence, the temperature and pressure dependence and quenching bymolecular dioxygen of which are reported for 2. The latter is attributed to energy transfer from the ⁴T₁ state exciting dioxygen to its ⁱΣ⁺ᵍ state and is responsible for the photosynthesis of the [(ThiaSO₂)(MnIII)(DMF)₂]Na (3) complex in DMF solution from 1 or 2. This reaction was studied by UV/Visible and EPR spectroscopy. The molecular structure and EPR spectroscopy of 3 are also presented.

Keywords: Thiacalixarene; Luminescence; Photooxidation; Manganese

Publ.-Id: 28984

Strong and Selective Ni(II) Extractants Based on Synergistic Mixtures of Sulfonic Acids and Bidentate N-Heterocycles

Roebuck, J. W.; Bailey, P. J.; Doidge, E. D.; Fischmann, A. J.; Healy, M. R.; Nichol, G. S.; O'Toole, N.; Pelser, M.; Sassi, T.; Sole, K. C.; Tasker, P. A.

Bidentate 5,5ʹ-alkyl-3,3ʹ-bi-1H-pyrazole and 2-(5-alkyl-1H-pyrazol-3-yl)pyridine ligands, L⁵ and L⁶ , have been shown to be stronger synergists for the solvent extraction of Ni(II) from sulfate solutions by dinonylnaphthalene sulfonic acid (DNNSAH) than the structurally related tridentate ligand 2,6-bis-[5-n-nonylpyrazol-3-yl]pyridine, L¹ , previously reported by Zhou and Pesic. The bidentate ligands are highly selective, providing the option of sequential recovery of Ni(II) and Co(II) and rejection of other metals commonly found in the liquors resulting from the acidic sulfate leaching of laterite ores. They were the strongest synergists identified in a screening carried out on 18 types of bidentate and tridentate N-heterocyclic ligands, including the recently reported 2-(2ʹ-pyridyl)imidazoles, L⁹⁻¹¹ . X-ray crystal structures of Ni(II) complexes of model ligands for L⁵ and L⁶ , having t-butyl rather than long-chain alkyl groups and with 2-naphthalene sulfonate rather than DNNSA⁻ as counteranions, show that the [Ni(L)₃ ]²⁺ complexes form strong H-bonds from the pyrazolyl NH groups to the oxygen atoms of the sulfonate groups, an arrangement that will stabilize [Ni(L)₃ ·(DNNSA)₂ ] assemblies and shield their polar functionalities from diluent molecules of the water-immiscible phase. UV–visible spectra and mass spectrometry provide evidence for the strong synergists displacing all water molecules from the inner coordination sphere of the Ni(II) ions.

Keywords: Ni recovery; laterite processing; synergistic solvent extraction; outer-sphere bonding; supramolecular chemistry


Publ.-Id: 28983

Stationary beam full-field transmission helium ion microscopy using sub-50 keV He+: Projected images and intensity patterns

Mousley, M.; Eswara, S.; de Castro, O.; Bouton, O.; Klingner, N.; Koch, C. T.; Hlawacek, G.; Wirtz, T.

A dedicated Transmission Helium Ion Microscope (THIM) for sub-50 keV helium was developed to investigate ion scattering processes and contrast mechanisms to develop new imaging and analysis modalities. Unlike a commercial Helium Ion Microscope (HIM), the in-house built instrument allows full flexibility in experimental configuration. Here, we report transmission imaging and scattering patterns obtained from powder and bulk crystalline samples using a stationary broad-beam as well as convergent-beam illumination conditions in THIM. The scattered He+ ions formed unexpected spot patterns in the far-field for MgO, BN and NaCl powder samples, but not for Si bulk sample. The mechanistic origins of the spot patterns in these samples were investigated. Surface diffraction of ions was excluded as a possible cause because the recorded scattering angles do not correspond to the predicted Bragg angles. Complementary Secondary Electron (SE) imaging in a HIM revealed that these samples charge significantly under He+ ion irradiation. It is suggested that the spot patterns obtained in THIM experiments are artefacts related to sample charging. The results presented here indicate that factors other than channelling, blocking and surface diffraction of ions have an impact on the final scattered intensity distribution in the far-field. Hence, the different processes contributing to the final scattered intensities should be understood in more detail to decouple and study the relevant ion beam scattering phenomena.

Keywords: Helium Ion Microscopy; ion scattering; Transmission Ion Microscopy

Publ.-Id: 28982

Uranium(VI) Complexes of Glutathione Disulfide Forming in Aqueous Solution

Kretzschmar, J.; Strobel, A.; Haubitz, T.; Drobot, B.; Steudtner, R.; Barkleit, A.; Brendler, V.; Stumpf, T.

The interactions between glutathione disulfide, GSSG, the redox partner and dimer of the intracellular detoxification agent glutathione, GSH, and hexavalent uranium, U(VI), were extensively studied by solution NMR, complemented by time-resolved laser-induced fluorescence and IR spectroscopies. As expected for the hard Lewis acid U(VI), coordination facilitates by the ligands’ O-donor carboxyl groups. However, owing to the adjacent cationic α-amino group, the glutamyl-COO reveal monodentate binding, while the COO of the glycyl residues show bidentate coordination. The log K value for the reaction UO₂2+ + H₃GSSG = [UO₂H₃GSSG]+ (pH 3, 0.1 M NaClO₄) was determined for the first time, being 4.81 ± 0.08; extrapolation to infinite dilution gave log K° = 5.24 ± 0.08. U(VI) and GSSG form precipitates in the whole pD range studied (2 – 8), showing least solubility for 4 < pD < 6.5. Thus, particularly GSSG, hereby representing also other peptides and small proteins, affects the mobility of U(VI), strongly depending on the speciation of either component.

Keywords: uranium; uranyl; U(VI); glutathione; GSH; glutathione disulfide; GSSG; oxidized glutathione; complex; NMR; TRLFS; FT-IR; spectroscopy; stability constant


Publ.-Id: 28981

Dimeric and Trimeric Uranyl(VI)–Citrate Complexes in Aqueous Solution

Kretzschmar, J.; Tsushima, S.; Lucks, C.; Jäckel, E.; Meyer, R.; Steudtner, R.; Müller, K.; Roßberg, A.; Schmeide, K.; Brendler, V.

This research addresses a subject discussed controversially for almost 70 years. The interactions between the uranyl(VI) ion, U(VI), and citric acid, H₃Cit, were examined by a multi-method approach comprising NMR, UV-Vis, ATR FT-IR, and EXAFS spectroscopies as well as DFT calculations. Combining ¹⁷O NMR and DFT calculation allowed an unambiguous decision on complex configurations, evidencing for the first time that the dimeric complex, (UO₂)₂(HCit–H)₂², exists as two diastereomers, with the syn isomer in aqueous solution strongly favored over the anti isomer. Both isomers interconvert mutually, with exchange rates of ~30 s¹ at −6 °C and ~249 s¹ at 60 °C in acidic solution, corresponding to an activation barrier of about 24 kJ mol¹. Upon increasing pH, ternary dimeric mono- and bis-hydroxo as well as trimeric complexes form, i.e. (UO₂)₂(HCit–H)₂(OH)³, (UO₂)₂(HCit–H)₂(OH)₂⁴, (UO₂)₃(O)(Cit–H)₃⁸, and (UO₂)₃(O)(OH)(Cit–H)₂⁵, respectively. Stability constants were determined for all dimeric and trimeric species, with log β° = −(8.6 ± 0.2) for the 3:3 species being unprecedented. Additionally, in the 6:6 sandwich complex, formed from two units 3:3 species, the ¹⁷O NMR resonance of the trinuclear uranyl(VI) core bridging µ₃-O is shown for the first time. Species distribution calculations suggest that the characterized polynuclear uranium(VI)-citate species do not significantly increase uranium(VI) mobility in the environment. Furthermore, we revise the misconceptions in aqueous U(VI) citric acid solution chemistry, i.e. structures proposed and repeatedly taken up, and outline generalized isostructural considerations to provide a basis for future uranium(VI) complexation studies.

Keywords: uranium; uranyl; U(VI); citric acid; citrate; molecular structure; NMR; ATR FT-IR; UV-Vis; EXAFS; spectroscopy; ternary complex; uranium hydrolysis; stability constant; isomerization; NMR dynamics

Related publications


  • Secondary publication expected from 20.05.2022

Publ.-Id: 28980

Efficient calculation methods for the diffusion coefficient of interstitial solutes in dilute alloys

Wang, X.; Faßbender, J.; Posselt, M.

In the example of oxygen diffusion in dilute ferritic iron alloys it is shown that the calculation of the diffusion coefficient can be separated into a contribution related to the migration in the interaction region between oxygen and the substitutional solute and a part related to diffusion in pure bcc Fe. The corresponding diffusion times are determined by analytical expressions using Density-Functional-Theory (DFT) data for the respective binding energies. The diffusion coefficient in the interaction region must be determined by atomistic kinetic Monte Carlo (AKMC) simulations with DFT values for the migration barriers as inputs data. However, in contrast to previous calculations, AKMC simulation must be performed only for one concentration of the substitutional solute, and the obtained results can be employed to obtain data for other concentrations in a very efficient manner. This leads to a tremendous decrease of computational efforts. Under certain conditions it is even possible to use only analytical expression where merely DFT data for the binding energies are needed. The limits of applicability of the presented calculation procedures are discussed in detail. The methods presented in this work can be generalized to interstitial diffusion in other host materials with small concentrations of substitutional solutes.

Keywords: Diffusion coefficient; Interstitial solute; dilute alloy; Efficient calculation; First-principle calculations; Atomistic kinetic Monte Carlo simulations

  • Open Access Logo Materials 12(2019)9, 1491
    DOI: 10.3390/ma12091491
  • Lecture (Conference)
    EUROMAT 2019, 01.-05.09.2019, stockholm, sweden

Publ.-Id: 28979

Defects and mechanical properties in weakly damaged Si ion implanted GaAs

Creutzburg, S.; Schmidt, E.; Kutza, P.; Loetzsch, R.; Uschmann, I.; Undisz, A.; Rettenmayr, M.; Gala, F.; Zollo, G.; Boulle, A.; Debelle, A.; Wendler, E.

Damage formation is investigated in GaAs implanted with 1 MeV Si ions to ion fluences from 3 × 10¹² to 5 × 10¹⁵ cm⁻² at room temperature. Under the conditions applied, amorphization of the implanted layers does not occur. The weakly damaged layers are studied by applying different experimental techniques including Rutherford backscattering spectrometry in channeling configuration, x-ray diffraction, in situ curvature measurement, optical subgap spectroscopy, and transmission electron microscopy. The results are evaluated and quantitatively connected with each other. Damage formation is described as a function of the ion fluence using a common defect evolution model. Point defects and defect clusters have to be taken into account in the ion fluence range of main interest up to 2 × 10¹⁵ cm⁻². Point defects contribute by a factor of about 8 more to both perpendicular strain and in-plane stress than defect clusters. When the concentration of point defects or the induced strain reaches a critical value, defect clusters form, which ensures that no further increase of perpendicular strain occurs. This reveals a clear driving force for cluster formation. The microstructure of the defect clusters cannot be determined from the results. As₃Ga₂ interstitial clusters are supposed. A remarkable decrease of the shear modulus of the implanted layers below the value of pristine GaAs by ≈ −35% is observed. Surprisingly, the change of shear modulus already sets in at a very low damage level of a few percent

Publ.-Id: 28978

Performance enhancement and characterization of liquid displacement battery having faradaic membrane

Mushtaq, K.; Zhao, J.; Weber, N.; Sadoway, D.

Übersicht über die Forschungsarbeiten zu "Liquid Displacement Batteries" am MIT, USA.

  • Poster
    14th Workshop on Reactive Metal Processing, 15.03.2019, Boston, USA

Publ.-Id: 28977

Compliance-current-modulated resistive switching with multi-level resistance states in single-crystalline LiNbO3 thin film

Pan, X.; Shuai, Y.; Wu, C.; Luo, W.; Sun, X.; Zeng, H.; Guo, H.; Yuan, Y.; Zhou, S.; Böttger, R.; Cheng, H.; Zhang, J.; Zhang, W.; Schmidt, H.

Resistive switching behavior of a ca. 600 nm thick single-crystalline LiNbO3 (LNO) film has been investigated after vacuum-annealing. Oxygen vacancies (OVs) were generated in the LNO thin film during the annealing process. After electro-forming, filamentary resistive switching has been observed, and the performance of switching can be tuned by the compliance current level. Multi-level resistance states including four different low resistance states, were realized by setting different compliance currents, revealing that both concentration of OVs within the conductive filament and the geometry of the conductive filament influence the switching behavior. The conduction mechanisms of the charge transport during switching is discussed based on the current-voltage curves.

Publ.-Id: 28976

Proton irradiation induced defects in β-Ga2O3: A combined EPR and theory study

Bardeleben, H.; Zhou, S.; Gerstmann, U.; Skachkov, D.; Lambrecht, W.; Ho, Q.; Deák, P.

Proton irradiation of both n-type and semi-insulating bulk samples of β-Ga2O3 leads to the formation of two paramagnetic defects with spin S = 1/2 and monoclinic point symmetry. Their high introduction rates indicate them to be primary irradiation induced defects. The first electron spin resonance (EPR1) has a g-tensor with principal values of gb = 2.0313, gc = 2.0079, and ga* = 2.0025 and quasi-isotropic superhyperfine interaction of 13G with two equivalent Ga neighbors. Under low temperature photoexcitation, this defect is quenched and replaced by a different metastable spin S = 1/2 center of comparable intensity. This second defect (EPR2) has similar principal g-values of gb = 2.0064, gc = 2.0464, and ga* = 2.0024 and shows equally superhyperfine interaction with two equivalent Ga atoms. This EPR2 defect is stable up to T = 100 K, whereas for T > 100 K the initial defect is recovered. Density functional theory calculations of the spin Hamiltonian parameters of various intrinsic defects are carried out using the gauge including projector augmented wave method in order to determine the microscopic structure of these defects. The intuitive models of undistorted gallium monovacancies or self-trapped hole centers are not compatible with neither of these two defects.

Publ.-Id: 28975

Double-peak specific heat and spin freezing in the spin-2 triangular lattice antiferromagnet FeAl2Se4

Li, K.; Jin, S.; Guo, J.; Xu, Y.; Su, Y.; Feng, E.; Liu, Y.; Zhou, S.; Ying, T.; Li, S.; Wang, Z.; Chen, G.; Chen, X.

We report the properties of a triangular lattice iron-chalcogenide antiferromagnet FeAl2Se4.The spin susceptibility reveals a significant antiferromagnetic interaction with a Curie-Weiss temperature Θ_CW≃−200K and a spin-2 local moment. Despite a large spin and a large ∣Θ_CW∣, the low-temperature behaviors are incompatible with conventional classical magnets. No long-range order is detected down to 0.4 K. Similar to the well-known spin-1 magnet NiGa2S4, the specific heat of FeAl2Se4 exhibits a double-peak structure and a T2 power law at low temperatures, which are attributed to the underlying quadrupolar spin correlations and the Halperin-Saslow modes, respectively. The spin freezing occurs at ∼14 K, below which the relaxation dynamics is probed by the ac susceptibility. Our results are consistent with the early theory for the spin-1 system with Heisenberg and biquadratic spin interactions. We argue that the early proposal of the quadrupolar correlation and gauge glass dynamics may be well extended to FeAl2Se4. Our results provide useful insights about the magnetic properties of frustrated quantum magnets with high spins.


Publ.-Id: 28974

Oxyhydride Nature of Rare-Earth-Based Photochromic Thin Films

Cornelius, S.; Colombi, G.; Nafezarefi, F.; Schreuders, H.; Heller, R.; Munnik, F.; Dam, B.

Thin films of rare-earth (RE)−oxygen−hydrogen compounds prepared by reactive magnetron sputtering show a unique color-neutral photochromic effect at ambient conditions. While their optical properties have been studied extensively, the understanding of the relationship between photochromism, chemical composition, and structure is limited. Here we establish a ternary RE−O−H composition-phase diagram based on chemical composition analysis by a combination of Rutherford backscattering and elastic recoil detection. The photochromic films are identified as oxyhydrides with a wide composition range described by the formula REOxH3−2x where 0.5 ≤ x ≤ 1.5. We propose an anion-disordered structure model based on the face-centered cubic unit cell where the O2− and H− anions occupy tetrahedral and octahedral interstices. The optical band gap varies continuously with the anion ratio, demonstrating the potential of band gap tuning for reversible optical switching applications.

Publ.-Id: 28973

Extension of the nodal code DYN3D to SFR applications

Nikitin, E.

DYN3D is a well-established Light Water Reactor (LWR) simulation tool and is being extended for safety analyses of Sodium cooled Fast Reactors (SFRs) at the Helmholtz-Zentrum Dresden-Rossendorf. This thesis focuses on the first stage of the development process, that is, the extension and application of DYN3D for steady-state and transient SFR calculations on reactor core level. In contrast to LWRs, the SFR behavior is especially sensitive to thermal expansions of the reactor components. Therefore, a new thermal-mechanical module accounting for thermal expansions is implemented into DYN3D. At first step, this module is capable of treating two important thermal expansion effects occurring within the core, namely axial expansion of fuel rods and radial expansion of diagrid. In order to perform nodal calculations with DYN3D, pre-generated homogenized few-group cross sections (XS) are necessarily needed. Therefore, prior to the development of thermal expansion models, a general methodology for XS generation is established for SFR nodal calculations based on the use of the Monte Carlo code Serpent. The new methodological developments presented in this thesis are verified against the Monte Carlo solutions of Serpent. Two SFR cores are used for testing: the large oxide core of the OECD/NEA benchmark and a smaller core from the Phenix end-of-life tests. Finally, the extended DYN3D is validated against selected IAEA benchmark tests on the Phenix end-of-life experiments that contain both steady-state and transient calculations. The contribution to the SFR-related developments at the HZDR, as presented in this thesis, makes it possible of performing steady-state and transient calculations for SFRs on reactor core level by using DYN3D. With this study, the basis of the next stage of DYN3D developments is established, that is, the up-scale of SFR analysis to system level can continue by coupling with a sodium capable thermal-hydraulic system code.

Keywords: SFR; thermal expansion; group constant generation; nodal methods; spatial kinetics; Monte Carlo; Serpent; DYN3D


Publ.-Id: 28972

Source term calculation and validation for F-18 production with a cyclotron for medical applications at HZDR

Konheiser, J.; Müller, S. E.; Magin, A.; Naumann, B.; Ferrari, A.

In this document we present the calculation and experimental validation of a source term for F-18 production with a cyclotron for medical applications operating at 18 MeV proton energy and 30 microA proton current. The Monte Carlo codes MCNP6 and FLUKA were used for the calculation of the source term. In addition, the radiation field around the O-18 enriched water target was simulated with the two codes. To validate the radiation field obtained in the simulation, an experimental program has been started using activation samples which are placed close to the water target during an F-18 production run of the cyclotron. After the irradiation, the samples are analyzed and the resulting activation is compared to Monte Carlo calculations of the expected sample activation. We and good agreement between simulations and experimental results, with most calculation to experiment (C/E) ratios well between 0.6 and 1.4.

Keywords: F-18; MCNP; FLUKA; Source Term; Cyclotron

Related publications

Publ.-Id: 28971

Fast-neutron-induced fission cross section of Pu(242) measured at the neutron time-of-flight facility nELBE

Kögler, T.

This dataset includes the processed data of the fast neutron-induced fission of Pu(242) experiement performed in November 2014 at the neutron time-of-flight facility nELBE which was published in T. Kögler et al., Phys. Rev. C 99, 024604

It contains the absolute (Pu242_nfis_Koegler_2019.csv) and relative (Pu242_U235_nfis_Koegler_2019.csv) cross section data ranging from 0.5 MeV to 10 MeV. The cross section data is given in comma separated ASCII files, as well as in a MS Excel-Sheet.

The columns of the tables are defined as follows:

  1. EN...neutron kinetic energy from the measured time of flight (ToF)
  2. EN-ERR...uncertainty of neutron kinetic energy = 0.5*(ToF bin width) = 1 ns
  3. DATA...cross section data
  4. ERR-S...statistical uncertainty of the cross section data
  5. ERR-SY...systematic uncertainty of the cross section data
  6. ERR-T...combined standard uncertainty of the cross section data
  7. ERR-0...relative uncertainty counting
  8. ERR-1...relative uncertainty normalization
  9. ERR-2...relative uncertainty reference cross section
  10. ERR-3...relative uncertainty FF detection inefficiency
  11. ERR-4...relative stat. uncertainty scattering correction H19
  12. ERR-5...relative sys. uncertainty scattering correction H19
  13. ERR-6...relative stat. uncertainty scattering correction PuFC
  14. ERR-7...relative sys. uncertainty scattering correction PuFC

Additionally, a root (see file is supplied, including the determined cross sections and all nessessary data to reconstruct the experiment. This includes the measured quantities, reference data, correction factors, evaluated cross sections etc.

To have the whole functionality of the root file, additional libary files ( and libGo4UserAnalysis_rdict.pcm) are also given here.

Keywords: neutron-induced fission; plutonium-242; cross section measurements; nuclear reactions; nucleon induced nuclear reactions; nELBE

Related publications

  • Reseach data in the HZDR data repository RODARE
    Publication date: 2019-03-06
    DOI: 10.14278/rodare.117
    License: CC-BY-4.0


Publ.-Id: 28970

Supplementary Data: Spectral Control via Multi-Species Effects in PW-Class Laser-Ion Acceleration

Huebl, A.; Rehwald, M.; Obst-Huebl, L.; Ziegler, T.; Garten, M.; Widera, R.; Zeil, K.; Cowan, T. E.; Bussmann, M.; Schramm, U.; Kluge, T.

Supplementary materials for our paper "Spectral Control via Multi-Species Effects in PW-Class Laser-Ion Acceleration".

Additional high-resolution, raw HDF5 files using the openPMD standard (DOI:10.5281/zenodo.1167843) increase simulation output data to 4.7 TByte and are available from the corresponding author upon reasonable request. 

Keywords: LPA; laser-ion acceleration; TNSA; multi-species; cryogenic target; particle-in-cell

Related publications

  • Reseach data in the HZDR data repository RODARE
    Publication date: 2019-03-06
    DOI: 10.14278/rodare.115
    License: CC-BY-SA-4.0


Publ.-Id: 28969

Understanding the size effects on the electronic structure of ThO2 nanoparticles

Amidani, L.; Plakhova, T. V.; Romanchuk, A. Y.; Gerber, E.; Weiss, S.; Efimenko, A.; Sahle, C. J.; Butorin, S. M.; Kalmykovc, S. N.; Kvashnina, K. O.

Developing characterization techniques and analysis methods adapted to the investigation of nanoparticles (NPs) is of fundamental importance considering the role of these materials in many fields of research. The study of actinide based NPs, despite their environmental relevance, is still underdeveloped compared to that of NPs based on stable and lighter elements. We present here an investigation of ThO2 NPs performed with High-Energy Resolution Fluorescence Detected (HERFD) X-ray Absorption Near-Edge Structure (XANES) and with ab initio XANES simulations. Structural models of ThO2 NPs with sharp edges and corners reproduce the size effect observed in experimental data. Inspection of the simulations from Th atoms in the core and on the surface of the NP indeed demonstrates that the origin of the effect is the lowering of the number of coordinating atoms for Th at the surface of the NP. The sensitivity of HERFD XANES to the less coordinated atoms at the surface may be exploited to investigate surface interactions.

  • Open Access Logo Physical Chemistry Chemical Physics 21(2019)20, 10635-10643
    Online First (2019) DOI: 10.1039/C9CP01283D


Publ.-Id: 28968

Ion irradiation driven changes of magnetic anisotropy in ultrathin Co films sandwiched between Au or Pt covers

Mazalski, P.; Kurant, Z.; Sveklo, I.; Dobrogowski, W.; Fassbender, J.; Wawro, A.; Maziewski, A.

Modifications of magnetic anisotropy of 30 keV Ga + ion irradiated ultrathin Co films sandwiched between Au or Pt buffer and capping layers are investigated as a function of magnetic layer thickness, d Co , and the ion fluence, F. Maps (d Co , F) of saturation fields have been derived from local magnetooptical polar Kerr effect (PMOKE) measurements. The areas with increased remanent magnetization and/or saturation fields, which are directly related to the uniaxial anisotropy, adopt linear shapes for the two branches in the maps. They are very distinct, especially for the Pt/Co/Pt system irradiated at lower and higher fluence. Replacement of Pt with Au in the buffer layer results in minor influence on the magnetization properties of the irradiated trilayers. Au as a capping layer significantly decreases the anisotropy in the branch appearing at lower fluence. In the Au/Pt/Au sandwich, a severe reduction of induced anisotropy is observed in both branches. The proposed phenomenological model describing experimentally investigated magnetic anisotropies enables separation of surface and volume contributions to both branches of enhanced anisotropy.

Keywords: Chemical driving force demixing; Ion beam irradiation; Magnetooptics; Perpendicular magnetic anisotropy


Publ.-Id: 28967

Digital LLRF Operation using MicroTCA at ELBE

Gümüş, Ç.; Hierholzer, M.; Kuntzsch, M.; Pfeiffer, S.; Schmidt, C.; Steinbrück, R.; Zenker, K.

The upgrade of the Low Level RF (LLRF) system of the Electron Linac for beams with high Brilliance and low Emittance (ELBE) at Helmholtz-Zentrum Dresden-Rossendorf (HZDR) was accomplished in 2018 . Now a digital system based on MTCA.4 can be used instead of the analogue system, which is operated since almost 20 years.The digital LLRF controller is implemented on a FPGA. The parametrisation and monitoring of the controller is performed by a ChimeraTK server application. ChimeraTK is a control system and hardware interface tool kit, which among others can provide an OPC-Unified Architecture (OPC-UA) interface. On the one hand, this interface is used to integrate the digital LLRF into the existing ELBE control and machine protection system, that is based on a Siemens PLC (S7) infrastructure. On the other hand, it is used to implement different additional clients of the ChimeraTK server application, such as the ELBE human machine interface used by the operators (WinCC, SCADA) or expert panels (e.g. LabView or Python). An overview of the new system including hardware as well as software components is given. In addition, an amplitude and phase noise measurement of a superconducting RF module are presented.

  • Invited lecture (Conferences)
    5. Annual Matter and Technology Meeting, 05.-07.03.2019, Jena, Germany

Publ.-Id: 28966

SPECT-Untersuchungen mit dem 123 I-markierten Dopamintransporter-Liganden FP-CIT (DaTSCAN):DGN-Handlungsempfehlung (S1-Leitlinie)

Tatsch, K.; Buchert, R.; Bartenstein, P.; Barthel, H.; Boecker, H.; Brust, P.; Drzezga, A.; La Fougère, C.; Gründer, G.; Grünwald, F.; Krause, B.-J.; Kuwert, T.; Langen, K.-J.; Rominger, A.; Sabri, O.; Schreckenberger, M.; Meyer, P. T.

Die S1-Leitlinie soll bei der Indikationsstellung, Durchführung, Interpretation und Befundung von SPECT-Untersuchungen des Dopamintransporters (DAT) mit DaTSCANTM unterstützen.
Gegenüber der Vorgängerversion von 2007 berücksichtigt die vorliegende Aktualisierung und Überarbeitung die neuere wissenschaftliche Literatur, zwischenzeitlich veröffentlichte Guidelines der europäischen (EANM) und amerikanischen Fachgesellschaften (SNM), sowie die aktuelle Fassung der S3-Leitlinie „Idiopathisches Parkinson-Syndrom“ der Deutschen Gesellschaft für Neurologie. Zudem finden neue technische Möglichkeiten Berücksichtigung.

  • Nuklearmedizin 58(2019)1, 5-16

Publ.-Id: 28965

Source term calculation and validation for F-18 production with a cyclotron for medical applications at HZDR

Konheiser, J.; Mueller, S. E.; Magin, A.; Naumann, B.; Ferrari, A.

Data contained in Fig. 2 of the

Keywords: Cyclotron; Source term; MCNP6; FLUKA

Related publications

  • Reseach data in the HZDR data repository RODARE
    Publication date: 2019-03-04
    DOI: 10.14278/rodare.113
    License: CC-BY-4.0


Publ.-Id: 28964

CFD-based optimization of heat exchanger tube bundle arrangement for passive spent fuel pool cooling to ambient air

Unger, S.; Beyer, M.; Krepper, E.; Hampel, U.

The storage of spent fuel in actively cooled water pools is common practice in nuclear power plants. One possibility to improve the reliability and the economy of spent fuel storage is the substitution of active cooling components by passive heat transfer systems. Thereby, ambient air should be the ultimate heat sink. A major drawback of natural convection heat transfer to ambient is the low heat transfer coefficient. Thus, bundle heat exchangers with finned tube are commonly employed. In one of our previous studies an optimum fin design was derived for such a heat exchanger. In the present investigation this tube bundle arrangement was numerical analysed with respect to optimal tube bundle configuration, tube shape, longitudinal tube pitch, transversal tube pitch and tube row number. We found highest heat transfer performance for oval shaped tubes with an axis ratio of 1:2.1 in a staggered configuration, having longitudinal tube pitch of 73 mm, a transversal tube pitch of 52 mm and 4 tube rows.

  • Contribution to proceedings
    50th Annual Meeting on Nuclear Technology, 07.-08.05.2019, Berlin, Deutschland
    Proceedings of the 50th Annual Meeting on Nuclear Technology

Publ.-Id: 28963

Spectral Control via Multi-Species Effects in PW-Class Laser-Ion Acceleration

Huebl, A.; Rehwald, M.; Obst-Huebl, L.; Ziegler, T.; Garten, M.; Widera, R.; Zeil, K.; Cowan, T. E.; Bussmann, M.; Schramm, U.; Kluge, T.

Laser-ion acceleration with ultra-short pulse, PW-class lasers is dominated by non-thermal, intra-pulse plasma dynamics. The presence of multiple ion species or multiple charge states in targets leads to characteristic modulations and even mono-energetic features, depending on the choice of target material. As spectral signatures of generated ion beams are frequently used to characterize underlying acceleration mechanisms, thermal, multi-fluid descriptions require a revision for predictive capabilities and control in next-generation particle beam sources. We present an analytical model with explicit inter-species interactions, supported by extensive ab initio simulations. This enables us to derive important ensemble properties from the spectral distribution resulting from those multi-species effects for arbitrary mixtures. We further propose a potential experimental implementation with a novel cryogenic target, delivering jets with variable mixtures of hydrogen and deuterium. Free from contaminants and without strong influence of hardly controllable processes such as ionization dynamics, this would allow a systematic realization of our predictions for the multi-species effect.

Keywords: LPA; laser-ion acceleration; TNSA; multi-species; cryogenic target; particle-in-cell

Related publications

  • Poster
    Laser-Plasma Accelerator Workshop 2019, 06.-10.05.2019, Split, Kroatien
  • Open Access Logo Plasma Physics and Controlled Fusion 62(2020)12, 124003
    DOI: 10.1088/1361-6587/abbe33

Publ.-Id: 28962

Revealing the Nature of Photoluminescence Emission in Metal-Halide Double Perovskites

Zelewski, S. J.; Urban, J. M.; Surrente, A.; Maude, D. K.; Kuc, A.; Schade, L.; Johnson, R. D.; Dollmann, M.; Nayak, P. K.; Snaith, H. J.; Radaelli, P. G.; Kudrawiec, R.; Nicholas, R. J.; Plochocka, P.; Baranowski, M.

Double perovskite crystals such as Cs2AgBiBr6 are expected to overcome the limitation of classic hybrid organic-inorganic perovskite crystals related to the presence of lead and the lack of structural stability. Perovskites are ionic crystals in which the carriers are expected to strongly couple to lattice vibrations. In this work we demonstrate that the photoluminescence (PL) emission in Cs2AgBiBr6 is strongly influenced by the strong electron-phonon coupling. Combining photoluminescence excitation (PLE) and Raman spectroscopy we show that the PL emission is related to a color center rather than a band-to-band transition. The broadening and the Stokes shift of the PL emission from Cs2AgBiBr6 is well explained using a Franck-Condon model with a Huang-Rhys factor of S=11.7 indicating a strong electron-phonon interaction in this material.

  • Open Access Logo Journal of Materials Chemistry C 7(2019)27, 8350-8356
    Online First (2019) DOI: 10.1039/C9TC02402F


Publ.-Id: 28961

Effect of four lanthanides onto the viability of two mammalian kidney cell lines

Heller, A.; Barkleit, A.; Bok, F.; Wober, J.

Exposure to lanthanides (Ln) poses a serious health risk to animals and humans. Since Ln are mainly excreted with the urine, we investigated the effect of La, Ce, Eu, and Yb exposure on renal rat NRK-52E and human HEK-293 cells for 8, 24 and 48 h in vitro. Cell viability studies using the XTT assay and microscopic investigations were combined with solubility and speciation studies using ICP-MS and TRLFS. Thermodynamic modeling was applied to predict the speciation of Ln in the cell culture medium. All Ln show a concentration- and time-dependent effect on both cell lines with Ce being the most potent element. In cell culture medium, the Ln are completely soluble and most probably complexed with proteins from fetal bovine serum. The results of this study underline the importance of combining biological, chemical, and spectroscopic methods in studying the effect of Ln on cells in vitro and may contribute to the improvement of the current risk assessment for Ln in the human body. Furthermore, they demonstrate that Ln seem to have no effect on renal cells in vitro at environmental trace concentrations. Nevertheless, especially Ce has the potential for harmful effects at elevated concentrations observed in mining and industrial areas.

Keywords: f-elements; renal cells; cytotoxicity; XTT; time-resolved laser-induced fluorescence spectroscopy; thermodynamic modeling

Publ.-Id: 28960

Magmatic vs. hydrothermal - origin of parisite-hosted REE mineralization at Nam Xe, Vietnam.

Heinig, T.; Möckel, R.; Krause, J.; Gutzmer, J.; Phan Quang, V.; Burisch, M.

The REE mineralization of Nam Xe, Vietnam, provides important new insights into paragenically complex carbonatite-related REE mineral formation associated with the transition from magmatic to hydrothermal conditions. Carbonatite dykes at Nam Xe comprise of calcite, ankerite and barite; these are crosscut by younger veins consisting of rare earth fluorcarbonates, fine-grained barytocelestine and calcite. The dominant rare earth fluorcarbonate is parisite [(REE)2Ca(CO3)3F2] with only minor bastnäsite and synchysite. Petrographic observations reveal that REE-mineralization is polystadial. Early bastnäsite associated with the magmatic stage is subsequently replaced by parasite in the presence of a Ca-CO3-rich carbothermal fluid. Parisite is then again overprinted by a Sr- rich hydrothermal fluid resulting in the formation of REE-enriched parisite and calcite.

Keywords: Rare earth fluorcarbonates; parisite; bastnäsite; carbonatite

  • Lecture (Conference)
    15th Biennial Meeting of the Society for Geology Applied to Mineral Deposits, 27.-30.08.2019, Glasgow, Scotland

Publ.-Id: 28959

Improved axial plane distance and velocity determination for ultrafast electron beam X-ray computed tomography

Neumann, M.; Bieberle, M.; Wagner, M.; Bieberle, A.; Hampel, U.

Ultrafast electron beam X-ray computed tomography (UFXCT) has in recent years become an indispensable tool for multiphase flow studies. An essential feature of this technique is fast cross-sectional imaging in two distinct planes. Both the spatial location of focal spot path and detectors as well as the angular scanning range in UFXCT differ from that of conventional X-ray CT systems. This brings in a spatial dependence in axial scanning position and resolution. In this paper, we present an analysis of this problem, which results in an improved description of the location and shape of the imaging regions, a more accurate map of the distance between the imaging planes and finally a higher precision in the determination of axial structure velocities. The benefit of this improved approach is exemplarily demonstrated for a two-phase pipe flow around an obstacle.

Keywords: ultrafast X-ray computed tomography; phase velocity measurement


Publ.-Id: 28958

Transparent Conductive Tantalum Doped Tin Oxide as Selectively Solar-Transmitting Coating for High Temperature Solar Thermal Applications

Lungwitz, F.; Escobar-Galindo, R.; Janke, D.; Schumann, E.; Wenisch, R.; Gemming, S.; Krause, M.

The transparent conductive oxide (TCO) SnO2:Ta is developed as a selectively solar-transmitting coating for concentrated solar power (CSP) absorbers. Upon covering with an antireflective layer, a calculated absorptivity of 95 % and an emissivity of 30 % are achieved for the model configuration of SnO2:Ta on top of a perfect black body (BB). High-temperature stability of the developed TCO up to 1073 K is shown in situ by spectroscopic ellipsometry and Rutherford backscattering spectrometry. The universality of the concept is demonstrated by transforming silicon and glassy carbon from non-selective into solar-selective absorbers by depositing the TCO on top of them. Finally, the energy conversion efficiencies of SnO2:Ta on top of a BB and an ideal non-selective BB absorber are extensively compared as a function of solar concentration factor C and absorber temperature TH. Equal CSP efficiencies can be achieved by the TCO on BB configuration with approximately 50 % lower solar concentration. This improvement could be used to reduce the number of mirrors in a solar plant, and thus, the levelized costs of electricity for CSP technology.

Keywords: concentrated solar power; solar thermal electricity; solar-selective transmitter; transparent conductive oxide; high-temperature in situ characterization


Publ.-Id: 28957

Interstellar ⁶⁰Fe in Antarctica

Koll, D.; Korschinek, G.; Faestermann, T.; Gómez-Guzmán, J.; Kipfstuhl, S.; Merchel, S.; Welch, J. M.

Earth is constantly bombarded with extraterrestrial dust containing invaluable information about extraterrestrial processes, e.g. structure formation by stellar explosions or nucleosynthesis, which could be traced back by long-lived radionuclides. Here, we report the very first detection of a recent ⁶⁰Fe influx on Earth by analyzing 500 kg of snow from Antarctica by Accelerator Mass Spectrometry. By the measurement of the cosmogenically produced radionuclide ⁵³Mn, an atomic ratio of ⁶⁰Fe/⁵³Mn=0.017 was found, significantly above cosmogenic production. After elimination of possible terrestrial sources, such as global fallout, the excess of ⁶⁰Fe could only be attributed to interstellar ⁶⁰Fe from the solar neighborhood.

Keywords: AMS; supernova; ⁶⁰Fe

Publ.-Id: 28955

Critical dynamics of the Kuramoto model on sparse random networks

Juhász, R.; Kelling, J.; Ódor, G.

We consider the Kuramoto model on sparse random networks such as the Erdős-Rényi graph or its combination with a regular two-dimensional lattice and study the dynamical scaling behavior of the model at the synchronization transition by large-scale, massively parallel numerical integration. By this method, we obtain an estimate of critical coupling strength more accurate than obtained earlier by finite-size scaling of the stationary order parameter. Our results confirm the compatibility of the correlation-size and the temporal correlation-length exponent with the mean-field universality class. However, the scaling of the order parameter exhibits corrections much stronger than those of the Kuramoto model with all-to-all coupling, making thereby an accurate estimate of the order-parameter exponent hard. We find furthermore that, as a qualitative difference to the model with all-to-all coupling, the effective critical exponents involving the order-parameter exponent, such as the effective decay exponent characterizing the critical desynchronization dynamics show a non-monotonic approach toward the asymptotic value. In the light of these results, the technique of finite-size scaling of limited size data for the Kuramoto model on sparse graphs has to be treated cautiously.

Keywords: Networks; Kuramoto Model; Synchronization


Publ.-Id: 28954

Small-angle neutron scattering (SANS): Overview on principles and best practices

Bergner, F.; Ulbricht, A.

This talk provides an introduction into the method of small-angle neutron scattering (SANS), elements of good practice for the application and analysis as well as selected applications in the field of nuclear materials.

  • Lecture (Conference)
    OECD/NEA Nuclear Science Committee Preparatory meeting: Best practices for nuclear materials characterisation techniques, 11.-12.02.2019, Boulogne-Billancourt, France

Publ.-Id: 28953

Critical synchronization dynamics of the Kuramoto model on connectome and small world graphs

Ódor, G.; Kelling, J.

The hypothesis, that cortical dynamics operates near criticality also suggests, that it exhibits universal critical exponents which marks the Kuramoto equation, a fundamental model for synchronization, as a prime candidate for an underlying universal model. Here, we determined the synchronization behavior of this model by solving it numerically on a large, weighted human connectome network, containing 804092 nodes, in an assumed homeostatic state. Since this graph has a topological dimension d<4, a real synchronization phase transition is not possible in the thermodynamic limit, still we could locate a transition between partially synchronized and desynchronized states. At this crossover point we observe power-law--tailed synchronization durations, with τt≃1.2(1), away from experimental values for the brain. For comparison, on a large two-dimensional lattice, having additional random, long-range links, we obtain a mean-field value: τt≃1.6(1). However, below the transition of the connectome we found global coupling control-parameter dependent exponents 1<τt≤2, overlapping with the range of human brain experiments. We also studied the effects of random flipping of a small portion of link weights, mimicking a network with inhibitory interactions, and found similar results. The control-parameter dependent exponent suggests extended dynamical criticality below the transition point.

Keywords: networks; brain; synchronization; kuramoto model

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Publ.-Id: 28952

Framework modifications and dehydration path of a Ag+-modified, STI-type zeolite

Cametti, G.; Scheinost, A. C.; Giordani, M.; Churakov, S. V.

The effect of Ag+ incorporation into stellerite, a natural zeolite with STI framework type, was investigated by means of Single Crystal X-ray Diffraction (SC-XRD), Molecular Dynamics (MD) simulations and X-ray Absorption Fine Structure Spectroscopy (XAFS). At room temperature the complete exchange of the original extraframework ions with Ag+ provoked a distortion of the framework accompanied by symmetry reduction from orthorhombic Fmmm to monoclinic F2/m space group. Ag+ ions were strongly disordered, with occupancies ranging from 0.02 to 0.24, at partially-occupied sites within zeolitic cages. The combination of ab initio molecular dynamic simulations and XAFS spectroscopy suggested that Ag+ is coordinated by three water oxygens at 2.37 Å and by two framework oxygens at ca. 2.55 Å. The thermal stability was monitored in situ by SC-XRD (from 25 to 400°C) and by XAFS (from 25 to 650°C). Upon heating the structure transformed to three different topologies: B phase, D’ phase, observed here for the first time, and D phase. The unit-cell volume contracted from 4392.85(14) at room temperature to 3644.4(4) Å3, measured at 400°C. Possible Ag+ to Ag0 reduction could be excluded although the formation of Ag+-Ag+ clusters could not be unambiguously ruled out.

Keywords: zeolite; molecular dynamics; SC-XRD; XAFS; XANES; Ag


Publ.-Id: 28951

Directed Evolution and Engineering of Gallium-Binding Phage Clones—A Preliminary Study

Schönberger, N.; Zeitler, C.; Braun, R.; Lederer, F.; Matys, S.; Pollmann, K.

The phage surface display technology is a useful tool to screen and to extend the spectrum of metal-binding protein structures provided by nature. The directed evolution approach allows identifying specific peptide ligands for metals that are less abundant in the biosphere. Such peptides are attractive molecules in resource technology. For example, gallium-binding peptides could be applied to recover gallium from low concentrated industrial wastewater. In this study, we investigated the affinity and selectivity of five bacteriophage clones displaying different gallium-binding peptides towards gallium and arsenic in independent biosorption experiments. The displayed peptides were highly selective towards Ga3+ whereby long linear peptides showed a lower affinity and specificity than those with a more rigid structure. Cysteine scanning was performed to determine the relationship between secondary peptide structure and gallium sorption.
By site-directed mutagenesis, the amino acids of a preselected peptide sequence are systematically replaced by cysteines. The resulting disulphide bridge considerably reduces the flexibility of linear peptides. Subsequent biosorption experiments carried out with the mutants obtained from cysteine scanning demonstrated, depending on the position of the cysteines in the peptide, either a considerable increase in the affinity of gallium compared to arsenic or an increase in the affinity for arsenic compared to gallium. This study shows the impressive effect on peptide–target interaction based on peptide structure and amino acid position and composition via the newly established systematic cysteine scanning approach.

Keywords: phage surface display; gallium; metal–peptide interaction; site-directed mutagenesis; cysteine; peptide structure

Publ.-Id: 28950

Nuclear level densities and gamma-ray strength functions in samarium isotopes

Naqvi, F.; Simon, A.; Guttormsen, M.; Schwengner, R.; Frauendorf, S.; Reingold, C. S.; Burke, J. T.; Cooper, N.; Hughes, R. O.; Humby, P.; Koglin, J.; Ota, S.; Saastamoinen, A.

The gamma-strength functions and level densities of in the quasi-continuum of 147,149Sm isotopes have been extracted from particle-gamma coincidences using the Oslo method. The nuclei of interest were populated via (p,d) reactions on pure 148,150Sm targets and the reaction products were recorded by the HYPERION array. An upbend in the gSF has been observed. The systematic analysis of the gSF for a range of Sm isotopes show that the scissors mode and the upbend compete with each other. Shell model calculations show a very good agreement with the experimental gSFs and confirm the competition between the upbend and scissors mode.

Keywords: Nuclear structure; light-ion reactions; gamma spectroscopy; level densities; strength functions; shell-model calculations

Publ.-Id: 28949

A proof of principle experiment for microbeam radiation therapy at the Munich Compact Light Source

Dombrowsky, A. C.; Burger, K.; Porth, A.-K.; Stein, M.; Dierolf, M.; Günther, B.; Achterhold, K.; Gleich, B.; Feuchtinger, A.; Bartzsch, S.; Beyreuther, E.; Combs, S. E.; Pfeiffer, F.; Wilkens, J. J.; Schmid, T. E.

Microbeam radiation therapy (MRT), a preclinical form of spatially fractionated radiotherapy, uses an array of microbeams of hard synchrotron X-ray radiation. Recently, compact synchrotron X-ray sources got more attention as they provide essential prerequisites for the translation of MRT into clinics while overcoming the limited access to synchrotron facilities. At the Munich Compact Light Source (MuCLS), a beamline at one of these novel compact X-ray sources, a proof of principle experiment was conducted applying MRT to a xenograft tumor mouse model. First, subcutaneous tumors derived from the established squamous carcinoma cell line FaDu were irradiated at a conventional X-ray tube using broadbeam geometry to determine a suitable dose range for the tumor growth delay.
For irradiations at the MuCLS, FaDu tumors were irradiated with broadbeam and microbeam irradiation at integral doses of either 3 or 5 Gy and tumor growth delay was measured. Microbeams had a width of 50 µm and a center-to-center distance of 350 µm with peak doses of either 21 or 35 Gy. A dose rate of up to 5 Gy/min was delivered to the tumor. Both doses and modalities delayed the tumor growth compared to a sham-irradiated tumor. The irradiated area and microbeam pattern were verified by staining of the DNA double-strand break marker γH2AX. This study demonstrates for the first time that microbeam radiation therapy can be successfully performed in vivo at the MuCLS.

Keywords: MRT; microbeam; compact source; tumor; X-rays; growth delay

Publ.-Id: 28948

Time dependence of the bioassociation behavior of U(VI) and Eu(III) with Brassica napus cells

Jessat, J.; Sachs, S.; Moll, H.; Steudtner, R.; Bok, F.; Stumpf, T.

For both the remediation of contaminated sites and the safety assessment of nuclear waste repositories detailed knowledge about the transfer of radionuclides (RN) into the food chain is of central concern. The association of RN with plants and their interaction with released metabolites influences whose fate in the environment. We studied the time and concentration dependent bioassociation of U(VI) and Eu(III) as an analogue for trivalent actinides with Brassica napus cells. The aim was to determine the effect of both heavy metals on the cell viability and the influence of the cell metabolism on the speciation and bioavailability of both metals. Due to the exposure of the cells with Eu(III) and U(VI) a time and concentration dependent bioassociation behavior was observed. At 200 µM U(VI) a multistage bioassociation process occurred resulting in a detachment of bioassociated U(VI) back into the medium. This change in the U(VI) speciation in the medium was observed by time-resolved laser-induced fluorescence spectroscopy. The occurrence of three different U(VI) species in the medium over the exposure time (Fig. 1) indicates the release of plant cell metabolites, that can act as ligands for U(VI) complexation and may impact its transfer in the environment. Model calculations for the speciation of U(VI) in the initial medium were performed on basis of the literature [1]. In order to identify possible plant cell metabolites, experiments on the enrichment and chromatographic separation of metabolites were carried out. In addition, the U(VI) complexation by relevant metabolites was studied.

[1] Sachs (2017) Environ. Sci. Technol. 51, 10843-10849.

Keywords: brassica napus; spectroscopy; species; TRLFS; bioassociation; metabolite; plant cells; Uranium; Europium

  • Poster
    Goldschmidt 2019, 18.-23.08.2019, Barcelona, Spain
  • Lecture (Conference)
    Goldschmidt 2019, 18.-23.08.2019, Barcelona, Spain

Publ.-Id: 28947

In vitro and in vivo Human Metabolism of (S)-[18F]Fluspidine – a Radioligand for Imaging σ1 Receptors with Positron Emission Tomography (PET)

Ludwig, F.-A.; Fischer, S.; Houska, R.; Hoepping, A.; Deuther-Conrad, W.; Schepmann, D.; Patt, M.; Meyer, P.; Hesse, S.; Becker, G.-A.; Zientek, F. R.; Steinbach, J.; Wünsch, B.; Sabri, O.; Brust, P.

(S)-[18F]fluspidine ((S)-[18F]1) has recently been explored for PET imaging of sigma-1 receptors in humans. In the current report, we have used plasma samples of healthy volunteers to investigate the radiometabolites of (S)-[18F]1 and elucidate their structures with LC-MS/MS. For the latter purpose additional in vitro studies were conducted by incubation of (S)-[18F]1 and (S)-1 with human liver microsomes (HLM). In vitro metabolites were characterized by interpretation of MS/MS fragmentation patterns from collision-induced dissociation or by use of reference compounds. Thereby, structures of corresponding radio-HPLC-detected radiometabolites, both in vitro and in vivo (human), could be identified. By incubation with HLM, mainly debenzylation and hydroxylation occurred, beside further mono- and di-oxygenations. The product hydroxylated at the fluoroethyl side chain was glucuronidated. Plasma samples (10, 20, 30 min p.i., n=5-6), obtained from human subjects receiving 250-300 MBq (S)-[18F]1 showed 97.2%, 95.4%, and 91.0% of unchanged radioligand, respectively. In urine samples (90 min p.i.) the fraction of unchanged radioligand was only 2.6% and three major radiometabolites were detected. The one with the highest percentage, also found in plasma, matched the glucuronide formed in vitro. Only a small amount of debenzylated metabolite was detected. In conclusion, our metabolic study, in particular the high fractions of unchanged radioligand in plasma, confirms the suitability of (S)-[18F]1 as PET radioligand for sigma-1 receptor imaging.

Keywords: Sigma-1 receptors (S1R); fluspidine; positron emission tomography (PET); radiometabolites; liquid chromatography-mass spectrometry (LC-MS); liver microsomes

Publ.-Id: 28946

Selective histone deacetylase inhibitors as prospective radiotracers for PET imaging

Clauß, O.; Scheunemann, M.; Hansen, F. K.; Brust, P.

The class I histone deacetylases (HDACs) 1, 2 and 3 are overexpressed in several types of cancer, neurodegenerative diseases and inflammation. The catalyzed deacetylation of lysine residues on histones represents a key epigenetic modification that modulates the chromatin and thus influence the gene expression and transcription. Inhibition of zinc-dependent HDACs relaxes the chromatin structure and can result in transcriptional activation and anticancer effects, e.g. induction of apoptosis. Consequently, radiolabelled HDAC inhibitors have emerged as a potential tool for the diagnostic imaging of tumors by positron emission tomography (PET).
The aim of this work is the development of novel highly affine and selective fluorine containing derivatives of a class I selective HDAC inhibitor to obtain the corresponding 18-fluorine PET radiotracers with an ortho-aminoanilide as zinc-binding motif for targeting class I HDACs in tumors. A series of fluorinated reference compounds will be synthesized and the binding affinities and selectivities towards the HDAC isoforms 1, 2 and 3 will be determined. Our strategy is mainly focused on the medicinal chemistry of fluorine-containing derivatives, which are suitable for direct and indirect nucleophilic radiofluorination. For the most promising compounds, precursors for radiolabeling will be synthesized and a fully automated procedure will be established. The evaluation of physicochemical properties, e.g. stability and lipophilicity of the radiolabelled compounds will be assessed and further in vitro and in vivo investigations performed.

Keywords: Histone deacetylase inhibitors; Positron emission tomography; Fluorinated compounds

  • Poster
    NCT Retreat 2019, 09.-10.05.2019, Heidelberg, Deutschland

Publ.-Id: 28945

Instability of precession driven Kelvin modes: Evidence of a detuning effect

Herault, J.; Giesecke, A.; Gundrum, T.; Stefani, F.

We report an experimental study of the instability of a nearly resonant Kelvin mode forced by precession in a cylindrical vessel. The instability is detected above a critical precession ratio via the appearance of peaks in the temporal power spectrum of pressure fluctuations measured at the end walls of the cylinder. The corresponding frequencies can be grouped into frequency sets satisfying resonance conditions with the forced Kelvin mode. We show that one set forms a triad that is associated with a parametric resonance of Kelvin modes. We observe a significant frequency variation of the unstable modes with the precession ratio, which can be explained by a detuning mechanism due to the slowdown of the background flow. By introducing a semianalytical model, we show that the departure of the flow from the solid body rotation leads to a modification of the dispersion relation of Kelvin modes and to a detuning of the resonance condition. The second frequency set includes a very low frequency and does not exhibit the properties of a parametric resonance between Kelvin modes. Interestingly, this frequency set always emerges before the occurrence of the triadic resonances, i.e., at a lower precession ratio, which implies that it may correspond to a different type of instability. We discuss the relevance of an instability of a geostrophic mode described by Kerswell [Kerswell, J. Fluid Mech. 382, 283 (1999)], although other mechanisms cannot be completely ruled out.

Keywords: Precession; Dynamo; DRESDYN


Publ.-Id: 28944

Limited importance of EphrinA1–ligand, Src kinase, and focal adhesion kinase in EphA2-mediated regulation of metastasis in Mel-Juso and A375 human melanoma cells

Neuber, C.; Herwig, N.; Pietzsch, J.; Belter, B.

EphA2 receptor tyrosine kinase fulfils various functions in the development of cancers. Here we analyzed how regulation of EphA2 receptor influences metastatic properties in human melanoma cells in vitro and lung metastasis in vivo. Further, we investigated whether the effects are mediated by Src kinase/focal adhesion kinase (FAK) signaling downstream of EphA2. Therefore, as model Mel-Juso and A375 melanoma cell lines showing different intrinsic EphA2 expression levels were used. To regulate EphA2 expression and activity, we used RNA interference, transgeneic EphA2 overexpression, and stimulation of EphA2 activity by adding EphrinA1. Adhesion to fibronectin was increased in EphA2-silenced cells and decreased in EphA2-overexpressing cells. Migration and planar motility were unaffected in Mel-Juso cells, but increased in EphA2-silenced A375 cells and decreased in EphA2-overexpressing A375 cells. Adhesion and migration were unaffected by EphrinA1-stimulation, indicating ligand-independent mechanisms. In vivo we detected increased lung metastasis in mice inoculated with EphA2-overexpressing Mel-Juso cells, substantiating the pro-metastatic effects of EphA2 in melanoma. Activity of Src kinase and FAK were unaffected in EphA2-silenced cells and in response to EphrinA1-stimulation. However, in EphA2-overexpressing A375 cells Src phosphorylation was increased, indicating enhanced Src activity. Together, these data suggest that EphA2 receptor promotes malignancy ligand-independently by mechanisms different from Src kinase/FAK signaling.

Keywords: Cellular adhesion; cellular migration; Eph receptor tyrosine kinases; Ephrins; malignant skin cancer; metastatic melanoma; RNA interference


  • Secondary publication expected

Publ.-Id: 28943

Regulation of A375 melanoma cell adhesion and migration by EphB4 and EphrinB2 –insights from co-culture experiments

Neuber, C.; Laube, M.; Mamat, C.; Belter, B.; Pietzsch, J.

BACKGROUND: Malignant melanoma is the most malignant skin neoplasm due to early metastasis and resistance to currently available therapies. Inflammatory tumor infiltrate, particularly macrophages, are of outstanding importance for melanoma progression and therapy response. EphB4 receptor and its preferred ligand EphrinB2 are also associated with melanoma progression, metastasis, and therapy resistance.
OBJECTIVE: The aim of our study was to systematically investigate the role of EphB4 for melanoma cell adhesion and migration, also in the presence of macrophages, considering experimental i) EphB4 overexpression, ii) EphB4 activation, iii) inhibition of EphB4 and EphrinB2 interaction, and iv) inhibition of EphB4 and downstream signaling.
RESULTS: Overexpression of EphB4 resulted in increased A375 melanoma cell adhesion showing EphrinB2 reverse signaling rather than EphB4 forward signaling being responsible. By contrast, A375 melanoma cell migration was not affected by EphB4 overexpression and effects due to modulation of EphB4/EphrinB2 signaling were inconsistent. In co-culture experiments macrophages (HL-60(M)) showed substantial influence on adhesion and migration of A375 cells. However, HL-60(M)-mediated effects could not be assigned to EphB4/EphrinB2 signaling but rather to cytokine signaling pathways.
CONCLUSIONS: Under the used experimental settings EphB4 is important for adhesion but not for the migration of A375 melanoma cells. Macrophages influenced adhesion and migration of melanoma cells but without significant involvement of EphB4/EphrinB2 signaling.

Keywords: Eph receptor tyrosine kinases; Ephrin ligands; malignant melanoma; metastasis; tumor microenvironment; tyrosine kinase inhibitors


  • Secondary publication expected

Publ.-Id: 28942

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