Publications Repository - Helmholtz-Zentrum Dresden-Rossendorf

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41396 Publications

Microbial mediated immobilization of radionuclide in a future crystalline nuclear-waste repository

Krawczyk-Bärsch, E.; Pedersen, K.; Arnold, T.; Bok, F.; Lehtinen, A.

The world’s first permanent nuclear-waste repository for high-level waste (HLW) will be the underground rock characterization facility tunnel ONKALO, situated near the nuclear power plants of Olkiluoto, approximately 300 km northwest of Helsinki (Finland). Geological mapping showed that the bedrock of the tunnel is mainly composed of veined gneisses with a migmatic appearance, which are interspersed by numerous fractures. Massive 5–10-mm thick biofilms (microbial communities) are observed attached to the tunnel walls where groundwater is seeping from bedrock fractures feeding the biofilm. Groundwater and biofilm samples were taken during the EURATOM collaborative project ReCosy for laboratory experiments in flow cells, where uranium(VI) was added to the circulating groundwater with a final uranium concentration (4.25×10–5 M), which was expected from a damaged and leaking waste canister in the far-field of a nuclear-waste repository. The aim of our studies was to simulate the fate and behaviour of uranium(VI) in the presence of microorganisms using different methods to find evidence of the possibility of uranium retention.

In our experiments, aqueous uranium percolated the biofilm and induced interaction between biofilm microorganisms and uranium(VI), forming an intracellular U-phosphate mineral similar to autunite (Ca[UO2]2[PO4]2 • 2-6H2O or meta-autunite Ca[UO2]2[PO4]2 • 10-12H2O) as determined by means of EF-TEM/EELS. The potential toxicity of uranyl was consequently avoided by the uranium forming these strong complexes with phosphate in the cytoplasm of these microorganisms. Inorganic phosphate (H2PO4–) was released from the cellular polyphosphate as a cells’ response to the heavy metal stress. In contrast, aqueous uranium carbonate species, likely calcium uranyl carbonates species (Ca2UO2[CO3]3), were formed using the large available amount of carbonate in the uranium-contaminated circulating groundwater. The results of the laser-induced fluorescence spectroscopy studies performed at 283 K are in excellent agreement with the thermodynamic calculations of the theoretical predominance fields of the uranium species formed in the uranium-contaminated circulating groundwater. These complexes consequently influence the speciation of uranium, contributing to the transport and migration of uranium(VI).

Our studies aimed to improve our understanding of the mechanisms by which biofilms respond to the exposure to radionuclide with respect to safety assessments in the far-field of nuclear-waste repositories. In this environment, microorganisms must be considered, along with minerals, as an important factor influencing radionuclide transport.

Keywords: uranium; biofilm; nuclear-waste repository

  • Poster
    EURADWASTE´13, 8th EC Conference on the Management of Radioactive Waste, 14.-16.10.2013, Vilnius, Lithuania
  • Contribution to proceedings
    EURADWASTE `13, 8th EC Conference on the Management of Radioactive Waste, 14.-16.10.2013, Vilnius, Lithuania

Permalink: https://www.hzdr.de/publications/Publ-18679
Publ.-Id: 18679


Pushing Plasma Simulations Towards Exascale Performance with PIConGPU

Bussmann, M.; Juckeland, G.

With PIConGPU, new physics phenomena previously not accessible within laser plasma simulations can be studied, which will help us optimize laser-driven radiation sources. Presents results on laser wakefield acceleration of electrons simulated on the Oakridge TITAN system and discuss in detail which techniques help us to get the most out of these clusters. Finally showing how to add fault-tolerance and load-balancing to a large hybridh CPU-GPU code such as PIConGPU to achieve optimum performance.

Keywords: gpu; particle-in-cell; pic; cuda; simulation

Related publications

  • Lecture (Conference)
    GPU Technology Conference (GTC), 18.-21.03.2013, San Jose, United States of America

Permalink: https://www.hzdr.de/publications/Publ-18678
Publ.-Id: 18678


PIConGPU - How to built one of the fastest GPU particle-in-cell codes in the world

Burau, H.; Debus, A.; Helm, A.; Hübl, A.; Kluge, T.; Widera, R.; Bussmann, M.; Schramm, U.; Cowan, T. E.; Juckeland, G.; Schmitt, F.; Nagel, W.

We present the algorithmic building blocks of PIConGPU, one of the fastest implementations of the particle-in-cell algortihm on GPU clusters. PIConGPU is a highly-scalable, 3D3V electromagnetic PIC code that is used in laser plasma and astrophysical plasma simulations.

Keywords: picongpu; particle-in-cell; pic; simulation; plasma; parallel; cuda

Related publications

  • Poster
    77. Jahrestagung der DPG und DPG-Frühjahrstagung, 04.-08.03.2013, Dresden, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-18677
Publ.-Id: 18677


Relativistic LTE fluid plasma simulation

Buikstra, L.; Bussmann, M.; van Goor, F.; Irman, A.; Schramm, U.; Cowan, T. E.

To allow simulation of nanosecond scale plasma processes, we are developing a 3D fully relativistic fluid code with LTE (local thermal equilibrium) closure. This code is intended to be able to take output from PIC simulations as its initial state, to allow self-consistent simulation of processes acting over multiple time and density scales. In this code, both electrons and ions are treated as inertial fluids. Local fluid pressure is tied to the energy density using the Maxwell-Jüttner distribution, allowing investigation of the effect of local temperatures on, for example, the expanding sheath in TNSA (target normal sheath acceleration) experiments.

Keywords: lte; plasma; fluid; simulation; tnsa

Related publications

  • Poster
    77. Jahrestagung der DPG und DPG-Frühjahrstagung, 04.-08.03.2013, Dresden, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-18676
Publ.-Id: 18676


Dynamics of ion heating and ionization in high power ultra-short laser pulses interacting with solid density plasmas

Huang, L.; Kluge, T.; Gutt, C.; Bussmann, M.; Cowan, T. E.

Plasma heating and ionization are important processes during the interaction of high power ultra-short laser pulses with solid density targets. In order to understand the relevant physics, particle-in-cell simulations including collisions and ionization were run to study ion heating dynamics in buried layer targets illuminated by high-intensity, ultra-short laser pulses. Our results show that bulk ions can be heated to above 1keV temperature. When studying the ionization dynamics strong filaments have been observed which depend on preplasma on the target front side, laser pulse duration and intensity. In order to study the evolution of ionization and ion bulk heating in experiment, ultra-bright X-ray free electron lasers - such as the European XFEL - are a very promising and strong tool to resolve the spatial and temporal scales of these processes inside the solid target.

Keywords: plasma; solid density; heating; buried layer; laser; simulation; xfel

Related publications

  • Lecture (Conference)
    77. Jahrestagung der DPG und DPG-Frühjahrstagung, 04.-08.03.2013, Dresden, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-18675
Publ.-Id: 18675


Hyperfine splitting in lithium-like bismuth

Lochmann, M.; Andelkovic, Z.; Botermann, B.; Bussmann, M.; Dax, A.; Frömmgen, N.; Hammen, M.; Hannen, V.; Jöhren, R.; Geppert, C.; Kühl, T.; Litvinov, Y.; Vollbrecht, J.; Nörtershäuser, W.; Stöhlker, T.; Thompson, R.; Volotka, A.; Weinheimer, C.; Wen, W.; Will, E.; Winters, D.; Sánchez, R.

High-precision measurements of the hyperfine splitting values on Li- and H-like bismuth ions, combined with precise atomic structure calculations allow us to test QED-effects in the regime of the strongest magnetic fields that are available in the laboratory. Performing laser spectroscopy at the experimental storage ring (ESR) at GSI Darmstadt, we have now succeeded in measuring the hyperfine splitting in Li-like bismuth. Probing this transition has not been easy because of its extremely low fluorescence rate. Details about this challenging experiment will be given and the achieved experimental accuracy will be presented.

Keywords: bismuth; li-like; spectroscopy; qed

Related publications

  • Lecture (Conference)
    DPG-Frühjahrstagung der Sektion AMOP (SAMOP), 18.-22.03.2013, Dresden, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-18674
Publ.-Id: 18674


Broadband lasercooling of relativistic ions at the ESR

Winters, D.; Clark, C.; Dimopoulou, C.; Giacomini, T.; Kozhuharov, C.; Kühl, T.; Lochmann, M.; Nörtershäuser, W.; Nolden, F.; Sanchez, R.; Sanjari, S.; Steck, M.; Stöhlker, T.; Ullmann, J.; Beck, T.; Birkl, G.; Rein, B.; Tichelmann, S.; Walther, T.; Ma, X.; Wen, W.; Yang, J.; Zhang, D.; Schramm, U.; Seltmann, M.; Siebold, M.; Bussmann, M.

We present new results on broadband laser cooling of stored relativistic C3+ ion beams at the ESR in Darmstadt. For the first time we could show laser cooling of bunched relativistic ion beams using a UV-laser which could scan over a very large range and thus cool all the ions in the ‘bucket’. This scheme is much more versatile than a previous scheme, where the bunching frequency was scanned relative to a fixed laser frequency. We have also demonstrated that this cooling scheme works without pre-electron cooling, which is a prerequisite for its general application to future storage rings and synchrotrons, such as the HESR and the SIS100 at FAIR. We also present results from in vacuo VUV-fluorescence detectors, which have proven to be very effective.

Keywords: laser cooling; ion beam; fair; esr

Related publications

  • Lecture (Conference)
    DPG-Frühjahrstagung der Sektion AMOP (SAMOP), 18.-22.03.2013, Hannover, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-18673
Publ.-Id: 18673


Broadband Lasercooling of Relativistic Ion Beams at ESR

Bussmann, M.; Seltmann, M.; Siebold, M.; Schramm, U.; Wen, W.; Winters, D.; Beck, T.; Rein, B.; Walther, T.; Tichelmann, S.; Birkl, G.; Sanchez-Alarcon, R.; Ullmann, J.; Lochmann, M.; Nörtershäuser, W.; Clark, C.; Kozhuharov, C.; Steck, M.; Dimopoulou, C.; Nolden, F.; Zhang, D.; Ma, X.; Stöhlker, T.; Sanjari, S.; Giacomini, T.; Yang, J.

We present new results on laser cooling of relativistic C3+ ion beams at the Experimental Storage Ring at GSI. For the first time we could show laser cooling of bunched relativistic ion beams using fast scanning of the frequency of the cooling laser over a range larger than the momentum acceptance of the bucket. Unlike previously employed cooling schemes where the bucket frequency was scanned relatively to a fixed laser frequency, scanning of the laser frequency can be readily applied to future high energy storage rings such as HESR or SIS 100 at FAIR.

Keywords: laser cooling; ion beam; esr

Related publications

  • Lecture (Conference)
    77. Jahrestagung der DPG und DPG-Frühjahrstagung, 04.-08.03.2013, Dresden, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-18672
Publ.-Id: 18672


PIConGPU - A Highly-Scalable Particle-in-Cell Implementation for GPU Clusters

Bussmann, M.; Burau, H.; Debus, A.; Hübl, A.; Kluge, T.; Pausch, R.; Schmeisser, N.; Schneider, B.; Steiniger, K.; Widera, R.; Wyderka, N.; Schramm, U.; Cowan, T. E.; Schmitt, F.; Grottel, S.; Gumhold, S.; Juckeland, G.; Nagel, W.

PIConGPU can handle large-scale simulations of laser plasma and astrophysical plasma dynamics on GPU clusters with thousands of GPUs. High data throughput allows to conduct large parameter surveys but makes it necessary to rethink data analysis and look for new ways of analyzing large simulation data sets. The speedup seen on GPUs enables scientists to add physical effects to their code that up until recently have been too computationally demanding. We present recent results obtained with PIConGPU, discuss scaling behaviour, the most important building blocks of the code and new physics modules recently added. In addition we give an outlook on data analysis, resiliance and load balancing with PIConGPU.

Keywords: gpu; particle-in-cell; pic; simulation

Related publications

  • Lecture (Conference)
    77. Jahrestagung der DPG und DPG-Frühjahrstagung, 04.-08.03.2013, Dresden, Deutschland
  • Lecture (Conference)
    DPG-Frühjahrstagung, 25.02.-01.03.2013, Jena, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-18671
Publ.-Id: 18671


Comparision of (-)-[18F]-Flubatine and 2-[18F]FA-85380 Binding to Nicotinic α4β2* Acetylcholine Receptors in Human Brains

Becker, G. A.; Wilke, S.; Schönknecht, P.; Patt, M.; Luthardt, J.; Hesse, S.; Meyer, P. M.; Barthel, H.; Sorger, D.; Seese, A.; Wagenknecht, G.; Hoepping, A.; Fischer, S.; Brust, P.; Sabri, O.

Aim:

Nicotinic α4β2* acetylcholine receptors (nAChR) are an important target for diagnostic neuroimaging because of their involvement in Alzheimer's disease, Parkinson's disease, tobacco and alcohol addiction. 2-[18F]FA-85380 (2-FA) has been used extensively for PET imaging of α4β2* receptors but is limited as biomarker by its unfavourable slow kinetic. The newly developed radiotracer (-)-[18F]-Flubatine (Flubatine) shows a significantly improved brain uptake, receptor affinity and selectivity (1). Here we estimated the compartmental parameters of both tracers by full kinetic modeling and compared them.

Materials and methods:

After intravenous administration of ~370 MBq radiotracer PET brain imaging was performed in 20 healthy controls with Flubatine (age 70.6±4.6, scan duration 90 min) and in 7 healthy controls with 2-FA (age 60.7±9.0, scan duration 420 min) using an ECAT EXACT HR+ system. PET frames were motion corrected with SPM2 and kinetic modeling using a 1-tissue compartment model (1TCM) with arterial input-function was applied to the volume of interest (VOI) based tissue time-activity curves (TACs) generated for 29 brain regions (anatomically defined via MRI co-registration). The model-based receptor parameter used was the total distribution volume VT (ml/cm3), tracer uptake was measured by K1 (ml/cm3/min) and tracer tissue clearance by k2 (1/min).

Results:

For both tracers TACs of all 29 brain regions could be described appropriately with the 1TCM and all kinetic parameters could be reliably estimated from the PET data. Regional VT increased as expected with regional nAChR density. Parameters of Flubatine in characteristic regions with very low, medium and high receptor density were: Corpus callosum (K1= 0.18±0.04, k2= 0.032±0.004, VT= 5.68±1.01), Frontal cortex (K1= 0.37±0.04, k2= 0.040±0.003, VT= 9.18±0.59), Thalamus (K1= 0.48±0.06, k2= 0.020±0.003, VT= 25.03±3.33). The respective parameters of 2-FA were: Corpus callosum (K1= 0.063±0.009, k2= 0.014±0.003, VT= 4.45±0.65), Frontal cortex (K1= 0.099±0.013, k2= 0.018±0.001, VT= 5.42±0.56), Thalamus (K1= 0.13±0.019, k2= 0.010±0.001, VT= 13.06±2.62).

Conclusions:

Flubatine is superior to 2-FA in tracer uptake velocity (characterized by K1), velocity of washout (characterized by k2) and in the amount of measured specific binding (characterized by VT-target - VT-reference). It shows a threefold higher uptake rate constant K1 and a twofold higher washout rate constant k2, providing the rational for much shorter scan durations in case of Flubatine. These results are in good agreement with our former findings in an animal (pig) model (1).

Reference:

1. P. Brust, ..O. Sabri: In vivo measurement of nicotinic acetylcholine receptors with [18F]Norchloro-Fluoro-Homoepibatidine (Flubatine). Synapse 2008;62:205-218.

  • Poster
    EANM 2013 - Annual Congress of the European Association of Nuclear Medicine, 19.-23.10.2013, Lyon, France, 19.-23.10.2013, Lyon, Frankreich
  • Abstract in refereed journal
    European Journal of Nuclear Medicine and Molecular Imaging 40(2013)2, S271-S271

Permalink: https://www.hzdr.de/publications/Publ-18670
Publ.-Id: 18670


Laser-driven Sources of Radiation Fundamentals, Simulations and Applications

Bussmann, M.

We present recent results on TNSA, simulations and laser cooling of ion beams

Keywords: tnsa; pic; gpu; picongpu; laser; cooling; ion; beam; acceleration

Related publications

  • Invited lecture (Conferences)
    XLIV. Arbeitstreffen "Kernphysik", 21.-28.02.2013, Schleching/obb., Deutschland

Permalink: https://www.hzdr.de/publications/Publ-18669
Publ.-Id: 18669


Scanner independent implementation of 3D list-mode reconstruction: proof of concep

Lougovski, A.; Domula, S.; Langner, J.; Hofheinz, F.; Schramm, G.; Steinbach, J.; van den Hoff, J.

Ziel/Aim:

Our aim was to port our previously developed high resolution 3D list-mode image reconstruction for the HR+ PET to the Philips Ingenuity TF PET/MR system. Porting to a different scanner usually requires a major rewrite to account for system specific aspects. Instead, a general interface was designed and implemented in our reconstruction to allow simultaneous support of multiple scanners and to facilitate future adoption to further scanner types. We report on application of this strategy for implementing our reconstruction on the Philips PET/MR.

Methodik/Methods:

We implemented a generalized interface using abstract classes which completely removes scanner dependency from the reconstruction algorithm and allows runtime switching between scanners. The reconstruction obtains system specific information
such as geometry parameters and data formats directly via an abstract interface using internal formats. The port to the Philips PET/MR was performed accordingly and evaluated: i) quantitative accuracy and spatial resolution in phantoms, ii) visual evaluation of patient studies, iii) runtime performance evaluation.

Ergebnisse/Results:

The use of an abstract interface influences the runtime performance of the reconstruction only minimal. The ported reconstruction shows substantial improvements in comparison to the vendor provided software. In phantoms we obtain improved resolution and a high level of quantitative accuracy. Visual inspection of phantom and patient data reveals an improved level of detail rendering.

Schlussfolgerungen/Conclusions:

The implementation of an abstract interface simplifies porting of the software to other scanners. For the Philips PET/MR we observed improved resolution and overall image quality compared to the vendor provided software. Support of Time-of-Flight information is currently implemented and already shows further improvements of image quality at reduced reconstruction times.

  • Poster
    51. Jahrestagung der Gesellschaft für Nuklearmedizin (DGN), 17.-20.04.2013, Bremen, Deutschland
  • Abstract in refereed journal
    Nuklearmedizin 52(2013), A81-A82
    ISSN: 0029-5566

Permalink: https://www.hzdr.de/publications/Publ-18668
Publ.-Id: 18668


Development and preparation of a novel carbon-11 containing radiotracer for non-invasive PET-Imaging of EphB4

Mamat, C.; Ebert, K.; Knieß, T.; Steinbach, J.

Ziel/Aim:

Members of the Eph receptor tyrosine kinase family play an essential role in the pathogenesis of cancer and, therefore, are promising candidates for molecular imaging purposes, e.g. by PET. In this regard, radiochemical access to 11C-radiotracers derived from potent inhibitors (IC50 = 1.3 nM, calcd. logP = 3.42) targeting EphB4 kinase domain and bearing the indazolylpyrazole structural motif was developed.

Methodik/Methods:

The evaluation of a protecting group strategy based on the ethoxyethyl moiety (EOE) was necessary for the regioselective labeling with [11C]CH3I due to three secondary amino groups of the precursor. The labeling was accomplished in a remotely controlled synthesis module in three steps. The first step involved the preparation of [11C]CH3I from [11C]CH4, the second step comprehended the radiolabeling of the protected precursor and the final step included the cleavage of the protecting group.

Ergebnisse/Results:

The synthesis of the reference as well as the precursor was done starting from EOE protected indazole. Subsequent reaction with 2,4-diochloropyrimidine give the first substructure. For the preparation of the precursor, the first substructure was treated with 3,5-di(morpholino)aniline under Buchwald-Hartwig conditions. For the preparation of the reference, the first substructure was first methylated and then treated with 3,5-di(morpholino)aniline. The radiolabeling was done starting with ~ 1-1.5 GBq [11C]CH3I under basic conditions. After 2 min reaction time 1 M HCl was added and the mixture was maintained for 2 min. Approx. 200 MBq of the desired radiotracer could be obtained within 20 min after EOB (30-35% d.c. yield based on [11C]CH4).

Schlussfolgerungen/Conclusions:

The two-step radiolabeling of a novel indazolylpyrazole derivative with [11C]CH3I was successfully demonstrated. First stability tests showed beneficial behaviour ex vivo. Further biological studies for an application as radiotracer for functional tumor imaging are ongoing.

Literatur/References:

Mamat C, Mosch B et al. (2012) ChemMedChem 7:1991-2003.

  • Poster
    51. Jahrestagung der Gesellschaft für Nuklearmedizin (DGN), 17.-20.04.2013, Bremen, Deutschland
  • Abstract in refereed journal
    Nuklearmedizin 52(2013), A72
    ISSN: 0029-5566

Permalink: https://www.hzdr.de/publications/Publ-18667
Publ.-Id: 18667


Application of the Huisgen reaction for the radiofluorination of SNEW peptides as probes for the Eph receptor monitoring

Mamat, C.; Pretze, M.; Bergmann, R.; Pietzsch, J.; Steinbach, J.

Ziel/Aim:

The synthesis of fluorine-18 labeled peptides with high affinity towards the EphB2 receptor and the evaluation as radiotracers for PET was described. This receptor is known to be overexpressed in various types of cancer. Thus, a peptide was applied with high affinity to the EphB2 receptor which is strongly constrained of the amino acid key sequence SNEW. Two novel bifunctional and bioorthogonal building blocks were evaluated. The labeling of the peptides was done using the Huisgen click approach.

Methodik/Methods:

Two labeling building blocks based on the piperazine skeleton with either alkyne or azide function were used and an automated module synthesis was evaluated. Further, it was found that the peptide SNEWILPRLPQH show a high affinity to EphB2. Thus, the C-terminus of the peptide was functionalized with alkyne or azide, to retain the high affinity which is constrained of the key sequence SNEW at the N-terminus.

Ergebnisse/Results:

The automated one-step radiosynthesis of two novel building blocks gave the desired piperazine derivatives [18F]AFP and [18F]BFP in radiochemical yields of 25-45% (d.c.) within 50 min and a high purity after convenient separation from [18F]F- and precursor using silica gel cardridges. Radiolabeling of several functionalized SNEW peptides under Click conditions pointed out that [18F]AFP is only suitable and yielded the radiofluorinated peptide in 10-15 % RCY (d.c.). A by-product was observed when the alkyne building block [18F]BFP was used due to the competing Glaser coupling. Finally, the peptide was prepared, radiolabeled and purified from the Cu with bispidine on SPPS. This is urgent, otherwise, aggreagtion of the peptide with Cu occur. Finally, the stability of the labeled SNEW peptide was investigated ex vivo showing >80% intact peptide after 1 h. Three more hydrophilic metabolites were observed not determined as [18F]F-.

Schlussfolgerungen/Conclusions:

With the SNEW peptides highly potent 18F-containing EphB2 inhibitors were found and the labeling on SPPS with [18F]AFP was successfully established.

  • Poster
    51. Jahrestagung der Gesellschaft für Nuklearmedizin (DGN), 17.-20.04.2013, Bremen, Deutschland
  • Abstract in refereed journal
    Nuklearmedizin 52(2013), A72
    ISSN: 0029-5566

Permalink: https://www.hzdr.de/publications/Publ-18666
Publ.-Id: 18666


Realistic simulations of laser-driven radiation sources. What we need and what is there.

Bussmann, M.

With upcoming supercomputer technology, the simulation of laser-driven radiation sources enters the realm of large-scale parameter surveys, interactive simulation and the possibility to add physical effects hitherto impossible to account for.
We present new ideas and techniques to deliver simulations that are closer to experiment and can be better connected to new experimental diagnostics.
We finally show how an integrated experimental and theoretical program is needed to increase the predictive capability of codes and why code validation will be the focus of laser plasma simulations.

Keywords: gpu; particle-in-cell; laser; acceleration; simulation; pic

Related publications

  • Invited lecture (Conferences)
    Institute Seminar MTA-PTE High-Field Terahertz Research Group, 07.02.2013, Pécs, Hungary

Permalink: https://www.hzdr.de/publications/Publ-18665
Publ.-Id: 18665


Festphasensynthese von selektiv mono-fluorbenzoylierten Polyaminen zur In-vivo-Adressierung von Transglutaminasen und Polyamin-Transportern

Wodtke, R.; Steinbach, J.; Pietzsch, J.; Löser, R.

Ziel/Aim:

Transglutaminasen und Polyamin-Transporter sind interessante Targets für die funktionelle Bildgebung von Tumoren mittels PET. Zur Adressierung dieser Targets sollen Polyamin-basierte Fluor-18-Tracer Anwendung finden, in denen das Radionuklid über die 4-Fluorbenzoylgruppe (FBz) eingeführt wird. Um die dafür erforderlichen Fluor-19-Analoga zugänglich zu machen, wurde eine Festphasensynthese entwickelt, die die selektive Fluorbenzoylierung an einer Aminogruppe in verschiedenen Polyaminen (u. a. Putrescin, Spermidin, Spermin) ermöglicht. Der etablierte Syntheseweg soll auf die entsprechenden F-18-markierten Analoga übertragen werden.

Methodik/Methods:

Zur selektiven mono-Fluorbenzoylierung wurde das von Wang et al. beschriebene Synthesekonzept angewendet (1). Es beinhaltet den Aufbau des Polyamin-Gerüstes durch Festphasensynthese der entsprechenden Oxopolyamine und deren anschließende Reduktion durch BH3/THF. Durch Einsatz von Dde und Boc als orthogonale Schutzgruppen und der Möglichkeit, mit 2-Acetyldimedon selektiv primäre Aminogruppen zu schützen, wird die selektive Fluorbenzoylierung verschiedener Aminogruppen ermöglicht.

Ergebnisse/Results:

Durch gezielte Anwendung des genannten Synthesekonzeptes konnten folgende neue Verbindungen in guten bis sehr guten Ausbeuten erhalten werden: N-FBz-Putrescin, N-FBz-Cadaverin, N1-FBz-3-Oxospermidin, N8-FBz-5-Oxospermidin, N1-FBz-3,8-Dioxospermin, N1-FBz-Spermidin, N4-FBz-Spermidin, N8-FBz-Spermidin und N1-FBz-Spermin. Die Identitäten der Verbindungen wurden NMR-spektroskopisch bestätigt.

Schlussfolgerungen/Conclusions:

Die Festphasensynthese mono-fluorbenzoylierter Polyamine und Oxopolyamine konnte erfolgreich etabliert werden. Durch das Vorliegen der Referenzverbindungen kann nun die Radiosynthese der Fluor-18-Analoga erfolgen, bei denen die 4-Fluorbenzoylgruppe [F-18]SFB-vermittelt angeknüpft wird. Dabei kann vermutlich analog zur Synthese der nichtradioaktiven Verbindungen vorgegangen werden.

Literatur/References:

(1) F. Wang, S. Manku, D. G. Hall, Org. Lett. 2000, 2, 1581-1583

  • Poster
    51. Jahrestagung der Gesellschaft für Nuklearmedizin (DGN), 17.-20.04.2013, Bremen, Deutschland
  • Abstract in refereed journal
    Nuklearmedizin 52(2013), A71
    ISSN: 0029-5566

Permalink: https://www.hzdr.de/publications/Publ-18664
Publ.-Id: 18664


Identification of Np(V) sorption complexes at the hematite-water interface studied by in-situ ATR FT-IR spectroscopy

Müller, K.; Gröschel, A.

Neptunium (Np) is one of the most important components of nuclear waste to consider for the long-term safety assessment of nuclear waste repositories, due to the increasing en-richment, the long half-life and the high toxicity of Np-237. Hence, great attention is attract-ed to its geochemistry [1]. Among the various geochemical reactions, the molecular pro-cesses occurring at the solid-water interface, e.g. sorption onto mineral phases, surface precipitation, and colloid formation strongly affect the migration behavior of the radioactive contaminant in the environment [2]. Thus, various components of geological materials, such as iron oxides and hydroxides play an important role in regulating the mobility of actinides in aquifers, due to their widespread environmental presence, high sorption capacity and tendency to form coatings on mineral surfaces [3]. In recent years, the sorption behavior of Np(V), the most relevant oxidation state under ambient conditions, onto iron oxides was mainly studied by macroscopic experiments [4]. For a better understanding of the molecular events occurring at the mineral’s surfaces, ATR FT-IR spectroscopy is a useful tool for the in-situ identification of surface species [5]. In addition, time-resolved measurements provide kinetic information on the surface reactions.
In this work, Np(V) sorption on hematite is studied under a variety of environmentally rele-vant sorption conditions by in-situ ATR FT-IR spectroscopy [5]. The IR spectra obtained from the subsequent steps of the experiment, that is (1) conditioning, (2) sorption, and (3) flushing, are shown in Fig. 1.
The absence of significant bands below 1000 cm−1 in the conditioning spectrum demon-strates the stability of the stationary hematite film directly prepared on the ATR crystal’s surface. The bands at 1491 and 1356 cm−1 represent the removal of carbonate by rinsing the hematite film, prepared in air with the CO2 free solution. Upon Np(V) sorption, the band observed at 790 cm−1 is assigned to the antisymmetric stretching vibrational mode (ν3) of the neptunyl ion. The IR spectrum obtained from an aqueous solution at 50 µM Np(V), 0.1 M, pH 6 shows the absorption of ν3(NpVO2) at 818 cm−1. The red shift of ν3 to 790 cm−1 upon sorption can be assigned to an inner-sphere monomeric sorption complex, as previ-ously reported for TiO2, SiO2 and ZnO [5]. The band at 1042 cm−1 is most probably due to surface modes of the mineral oxide provoked by the sorption processes and were already observed for interactions with U(VI), Cs(I) and CO32 [5]. In the flushing stage, a weakly bound species is released from the stationary phase, reflected by a negative band at 795 cm−1 in the respective spectra.
Additional experiments were performed at varied values of pH (5.6 – 12) and ionic strength (0.001 – 0.1) (Fig. 2). Upon increasing the pH from 5.6 to 8.6, no shifts of the bands at 1041 and 790 cm−1 are observed. But the intensities of these spectral features are consid-erably increased at higher pH values indicating an enhanced sorption capacity close to the IEP at pH 9.2. At pH > 10, the aqueous Np(V) speciation changes and NpO2OHaq is formed and distinctly changes the sorption behavior. The band of ν3(NpVO2) is shifted to 773 cm−1. The variation of ionic strength between 0.1 and 0.01 does not change the spectral characteristics. The higher intensities observed at 0.0001 M NaCl can be attributed to contributions of an outer-sphere complex which has to be verified by future experiments.
In summary, the IR spectra evidence the formation of Np surface complexes on hematite which can be easily removed to a considerable extent by flushing with blank solution. From this behavior, the simultaneous formation of an inner-sphere species with con-tributions of an outer-sphere complex is suggested.

[1] Kaszuba, J. P. et al. (1999) Environ. Sci. Technol. 33, 4427-4433.
[2] O'Day, P. A. (1999) Reviews of Geophysics 37, 249-274.
[3] Tochiyama, O. et al. (1996) Radiochim. Acta 73, 191-198.
[4] Brendler, V. et al. (2003) Journal of Contaminant Hydrology 61, 281-291.
[5] Müller, K. et al. (2009) Environ. Sci. Technol. 43, 7665-7670.

  • Contribution to proceedings
    Actinides 2013 - 9th International Conference on the Chemistry and Physics of the Actinide Elements, 21.-26.07.2013, Karlsruhe, Deutschland
    Proceedings of Actinides 2013
  • Lecture (Conference)
    Actinides 2013 - 9th International Conference on the Chemistry and Physics of the Actinide Elements, 21.-26.07.2013, Karlsruhe, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-18663
Publ.-Id: 18663


Verlaufsuntersuchung des periacetabulären Knochenstoffwechsel nach Hüft-Pfannenwechsel mittels Positronen-Emissions-Tomographie und F18-NaF (NaF-PET)

Beuthien-Baumann, B.; Bernstein, P.; Hofheinz, F.; Zessin, J.; Kotzerke, J.; Günther, K. P.

Ziel/Aim:

Die Revision von gelockerten Hüft-Pfannen kann den Einsatz von impaktierten Knochen-Allografts (CBA) zur Stabilisierung der Pfanne und zum Auffüllen von Knochendefekten erfordern. Können mittels NaF-PET osteometabolische Veränderungen des CBA zu einem frühen Zeitpunkt nach Revision dokumentiert werden?

Methodik/Methods:

18F-NaF-PETs wurde 1 und 6 Wochen nach Revision durchgeführt. 12 Patienten wurden in die Studie (BfS- und Ethik-Votum) eingeschlossen, 9 Patienten absolvierten PET1+2. Die PET wurden an einem ECAT EXACT HR+ (Siemens/ CTI, USA) durchgeführt. Nach einer 4-min. Transmissionsmessung (Ger-68-Stabquellen) begann mit i.v.-Injektion von 240– 300 MBq F18-NaF eine dynamische Emission über 30 min über den Hüften. Auf einem post-op CT wurden Volumes of interest (VOIs) abgegrenzt (CBA, supracetabulär, os pubis) und nach Fusion von CT- und PET-Datensätze auf das PET übertragen. Die quantitative NaF-Aufnahme der VOIs wurde mit einem irreversiblen 2-Kompartment-Modell berechnet. Die Inputfunktion wurde aus der A. iliaca communis der dynamischen PET bestimmt. Der Parameter km (min-1) repräsentiert den Fluorid-influx in den Knochen.

Ergebnisse/Results:

km des supracetabulären Knochen zeigte auf der operierten Seite von PET1 zu PET2 eine nicht signifikante Zunahme (mean (±SD)) von 0,0491 (±0,0249) auf 0,0678 (±0,0367). Das CBA zeigte eine nicht signifikante Zunahme von 0,0384 (±0,0307) auf 0,0549 (±0,0319). In Zusammenschau mit dem CT war diese Zunahme im Randbereich des CBA lokalisiert und konnte nicht sicher von angrenzendem genuinem Knochengewebe, das visuell bei PET2 eine höhere Stoffwechselaktivität aufwies, getrennt werden.

Schlussfolgerungen/Conclusions:

Die NaF-PET 1 und 6 Wochen nach Revision zeigt eine nicht signifikante Zunahme des Knochenstoffwechsels ipsilateral supracetabulär. In dem CBA können beginnende osteometabolische Veränderungen im Randbereich zum genuinen Knochen nicht ausgeschlossen werden, zur sicheren Dokumentation einer stabilen Durchbauung des CBA wäre eine NaF-PET zu einem späteren Zeitpunkt erforderlich.

  • Lecture (Conference)
    51. Jahrestagung der Gesellschaft für Nuklearmedizin (DGN), 17.-20.04.2013, Bremen, Deutschland
  • Abstract in refereed journal
    Nuklearmedizin 52(2013), A64
    ISSN: 0029-5566

Permalink: https://www.hzdr.de/publications/Publ-18662
Publ.-Id: 18662


Combined measurement of perfusion and glucose metabolism by PET/CT using O-15-water and F-18-fluorodeoxyglucose for improved tumor characterization in advanced cervical carcinoma

Apostolova, I.; Buchert, R.; Steffen, I. G.; Hofheinz, F.; Köhler, C.; Marnitz, S.; Brenner, W.

Ziel/Aim:

Therapy response varies considerably in advanced cervical carcinoma(ACC). Glucose metabolism and microvascular characteristics of the tumor have been evaluated as biomarkers for identification of patients with poor response before or early during treatment. The combination of both biomarkers for detection of tumor regions with a ‘malignant mismatch’(MM), i.e. strongly increased glycolysis at low blood flow levels, might indicate resistance to therapy. The aim of the present study was to test whether ACC show MM that can be detected by the combination of FDG- and O-15-water-PET.

Methodik/Methods:

Twelve women (27-69y) with locally ACC (FIGO IIB-IIIB; grade G2 n=7, G3 n=5) were included prior to chemo-radiation. Regional blood flow was computed voxel-by-voxel from the O-15-water PET using a weighted integral approach and an image-derived arterial input function. FDG uptake was characterized by SUV. The primary tumor was segmented manually in the CT. A tumor voxel was considered to present MM if the perfusion was lower than the median perfusion in the tumor and the SUV was higher than the median SUV. The absolute total MM volume (aMMV) was obtained by multiplying the number of MM voxels with the voxel volume. The relative MM volume (rMMV) was obtained by dividing the aMMV by the tumor volume.

Ergebnisse/Results:

The volumes of the primary tumors ranged from 54 to 225ml. The tumors were quite heterogeneous with respect to both FDG uptake and perfusion. The aMMV ranged from 7.7 to 35.5ml, the rMMV from 7.9 to 26.6%. There was no correlation between rMMV and tumor volume (p=0.517). T-testing revealed a tendency (p=0.083) for an association between aMMV and histological grading, aMMV being higher in the G3 than in the G2 tumors. There was no association between grading and rMMV (p=0.888).

Schlussfolgerungen/Conclusions:

ACC show a metabolism/perfusion MM to a strongly variable extent. The mismatch volume seems to be associated with the tumor grade. Evaluation of the prognostic value requires follow-up data in a larger cohort.

  • Lecture (Conference)
    51. Jahrestagung der Gesellschaft für Nuklearmedizin (DGN), 17.-20.04.2013, Bremen, Deutschland
  • Abstract in refereed journal
    Nuklearmedizin 52(2013), A54
    ISSN: 0029-5566

Permalink: https://www.hzdr.de/publications/Publ-18661
Publ.-Id: 18661


Fluor-18-Misonidazol-PET/CT unter kurativ intendierter Radiochemotherapie bei Patienten mit lokal fortgeschrittenen Kopf-Hals-Tumoren (KHT) – eine prospektive Explorationsstudie

Zöphel, K.; Zips, D.; Abolmaali, N.; Perrin, R.; Abramyuk, A.; Haase, R.; Appold, S.; Steinbach, J.; Baumann, M.; Kotzerke, J.

Ziel/Aim:

Hypoxie ist charakteristisch für solide Tumoren und trägt maßgeblich zu einem potenziellen Versagen einer Radiochemotherapie (RCT) bei. Ziel dieser prospektiven Studie war es deshalb, den prognostischen Wert der Hypoxie-Bildgebung vor und unter RCT bei Patienten mit lokal fortgeschrittenen Kopf-Hals-Tumoren (KHT) zu explorieren.

Methodik/Methods:

Fünfundzwanzig Patienten mit histologisch gesicherten, unbehandelten KHT im klinischen Stadium III / IV wurden mit der F-18-Misonidazol- (F-MISO-) PET/CT zu 4 Zeitpunkten der kurativ intendierten RCT (initial, 8-10 Gy, 18-20 Gy und 50-60 Gy) untersucht. Parameter wie die maximale Ziel-Hintergrund-Ratio und das Schwellwert-basierte Tumorvolumen bei verschiedenen Ziel-Hintergrund-Rationes, das Tumorvolumen aus der CT sowie typische Basisparameter der initial und bei 40 Gy durchgeführten FDG-PET/CT wurden zu allen Untersuchungszeitpunkten auf ihren prognostischen Wert hin untersucht. Als Endpunkt diente das lokal Progressions-freie Überleben (LPFS). In einer multivariaten Cox-Analyse (einschließlich klinischer Parameter) und mehreren Log-Rank-Tests erfolgte die Prüfung auf signifikante Unterschiede.

Ergebnisse/Results:

Die Parameter aus der F-MISO-PET zeigten eine Assoziation mit dem LPFS-Endpunkt, am strengsten assoziiert waren die Zeitpunkte bei 10 Gy und 20 Gy unter der RCT (p = 0,023-0,048 und 0,042-0,061 in der multivariaten Cox-Analyse). Parameter aus der initialen F-MISO-PET/CT waren nur in der univariaten Analyse signifikant. Weder klinische Parameter, noch CT- oder FDG-PET-basierte Tumorvolumina zeigten eine signifikante Assoziation mit dem LPFS.

Schlussfolgerungen/Conclusions:

Diese prospektive Explorationsstudie demonstriert die prognostische Bedeutung der F-MISO-PET/CT in der frühen Phase der kurativen RCT. F-MISO-Bilder nach 1 oder 2 Wochen RCT (bei 10 bzw. 20 Gy) sind vielversprechend, wenn es um die Selektion der Patienten geht, die von einer Modifikation der Hypoxie oder von einer Dosis-eskalierten Radiatio profitieren könnten. Eine prospektive Validierungsstudie läuft bereits.

  • Lecture (Conference)
    51. Jahrestagung der Gesellschaft für Nuklearmedizin (DGN), 17.-20.04.2013, Bremen, Deutschland
  • Abstract in refereed journal
    Nuklearmedizin 52(2013), A52-A53
    ISSN: 0029-5566

Permalink: https://www.hzdr.de/publications/Publ-18660
Publ.-Id: 18660


Investigating dust behaviour for safety

Barth, T.; Hampel, U.

The main purpose of Subproject 2 is to further investigate the Key Safety Aspects identified by the Safety Advisory Group of the RAPHAEL project and to contribute to their resolution. Work package 23 targets to fill the knowledge gaps in dust production, deposition and remobilisation. Experimental and (advanced) analytical methods have been adopted to investigate all aspects of dust behaviour.

Keywords: graphite dust; high temperature reactor; pebble bed; positron emission tomography

Permalink: https://www.hzdr.de/publications/Publ-18659
Publ.-Id: 18659


Imaging of α7 nicotinic acetylcholinereceptors (nAChRs): Automated synthesis and biological evaluation of [18F]NS14490 in mice and pig

Rötering, S.; Fischer, S.; Hiller, A.; Donat, C.; Scheunemann, M.; Peters, D.; Bergmann, R.; Ullrich, M.; Sabri, O.; Steinbach, J.; Deuther-Conrad, W.; Brust, P.

Aim
There is evidence that α7nAChRs play an important role in cancer and neurodegenerative diseases. Therefore, quantitative imaging of α7nAChRs using PET represents a new approach for investigation of those diseases.
Due to its high target affinity and selectivity [18F]NS14490, an oxadiazolyl-diazabicyclononane derivative, is a promising radiotracer for α7nAChRs imaging. Manual radiosynthesis of [18F]NS14490 and its in vivo evaluation in mice were already reported [1]. The subsequent assessment of its imaging potential by dynamic PET studies in piglets and PET/CT studies in tumor-bearing mice required the transfer of the manual synthesis to an automated synthesis module.

Materials and Methods
For dynamic PET studies, the manual radiosynthesis of [18F]NS14490 [1] was transferred to an automatic synthesis module (Tracerlab FX-N) including azeotropic drying of [18F]F- with Kryptofix K222/K2CO3 in acetonitrile, direct nucleophilic substitution at the precursor, semipreparative HPLC and solid phase extraction. After evaporation the radiotracer was formulated in phosphate buffered saline containing 5% ethanol.
Dynamic PET studies in piglets (female, 15-18 kg) were performed under control and blocking conditions (n=2 each) with a highly selective α7nAChRs ligand (NS6740; bolus: 3 mg kg-1 h-1; infusion: 1 mg kg-1 h-1) for 4 hours. The metabolism of [18F]NS14490 in piglets was analyzed by chromatography of plasma samples.
PET/CT studies were performed in tumor-bearing nude mice under control and blocking conditions with NS6740.

Results and Conclusion
During transfer of radiosynthesis into an automated synthesis module, solid phase extraction was challenging. For desorption of the radiotracer from divinyl/polystyrene cartridge, the elution solvent ethanol/acetic acid used in manual synthesis was replaced by acetonitrile/formic acid resulting in more efficient elution, formerly not accomplished. The radiotracer was achieved within 1.25 hours and radiochemical yields (32%), radiochemical purity (> 90%) and specific activity (> 150 GBq μmol-1) were comparable to the manual synthesis [1]. Brain uptake of [18F]NS14490 peaked in piglets at 3 min p.i. and is with a value of SUVmax = 0.504 about tenfold higher than in mice. Blocking by NS6740 decreased the specific uptake in brain by 28% (SUV 240 min p.i. 0.174 vs. 0.125 under baseline and blocking conditions, respectively).The metabolic stability of [18F]NS14490 in piglets is lower than in mice. At 60 min p.i. intact radiotracer represented 30% of plasma activity in piglets compared to 55% in mice.
Preliminary animal PET/CT studies in tumor-bearing mice provide evidence that [18F]NS14490 may also be suitable for tumor imaging.
[1] Rötering, S. et al. Bioorg. Med. Chem. 2013

  • Poster
    EANM 2013 - Annual Congress of the European Association of Nuclear Medicine, 19.-23.10.2013, Lyon, Frankreich
  • Abstract in refereed journal
    European Journal of Nuclear Medicine and Molecular Imaging 40(2013)2, S317-S317
    DOI: 10.1007/s00259-013-2535-3

Permalink: https://www.hzdr.de/publications/Publ-18658
Publ.-Id: 18658


Oxygen-18 water: Recycle?

Rötering, S.; Franke, K.; Brust, P.; Fischer, S.; Steinbach, J.

Aim
The standard method for fluorine-18 production relies on proton irradiation of oxygen-18 water. Increased demand and costs of O-18 water forced us to consider its re-use for research purposes. After irradiation and F-18 separation the target water is contaminated with radioactive metal ions and organic solvents disturbing its re-use. Therefore, thorough purification is needed before further irradiation is possible. Here, we present two methods for the removal of organic contaminants from used target water.

Materials and Methods
Two different methods were accomplished to oxidize the organic contaminants ethanol and acetone in O-18 water using photo-oxidation (Pen-Ray 254 nm, 5.4 W) [1] and a wet chemical method with KMnO4 and NaOH. Thereafter vacuum distillation was performed and the target water was validated by gas chromatography, ICP-OES, pH value, conductivity and pycnometry. In addition artificially contaminated O-16 water was used to evaluate the potential of both methods concerning the oxidation of other potential contaminants such as methanol and acetonitrile.
Target irradiations were performed at equal parameters of bombarding (beam current on target 35 μA, 11.7 μAh) at a CYCLONE 18/9 (IBA Molecular, Nirtra® Fluor L-target (99.9% niobium): 2 mL, target window: Havar alloy, 50 μm).
Radionuclide purity and yields were determined by gamma spectrometry (ORTEC) and an ionization chamber (MED Nuklear-Medizintechnik Dresden GmbH). Produced F-18 was used in nucleophilic substitution reactions in various radiosyntheses of ongoing projects.

Results and Conclusion
Using both purification methods a comparable decrease of organic contaminants from 400 μg mL-1 ethanol and 44 μg mL-1 acetone to 10 μg mL-1 – 50 μg mL-1 ethanol was achieved. Photo-oxidation was approximately 1.5times faster. Important parameters (amount of oxidation agent, temperature, treatment time) for both methods were defined to ensure reproducibility of the radiosyntheses after comparable proton irradiation as done for the purchased target water. We observed a loss of production yield (19%) compared to purchased water due to a lower O-18 concentration. No influence on radionuclide purity or radiochemical yields was observed. Both methods enable a multiple re-cycling of target water for successful F-18 production and application for research purposes. The re-cycling process is limited by the amount of F-18 required for radiosyntheses. Starting from 87% enrichment of O-18 in target water we found 83% enrichement after one cycle allowing reasonable production yields and efficient economical usage of the purchased target water including efforts to minimize the contamination of target water.
[1] DE 29504388 U1, 1995
:

  • Poster
    EANM 2013 - Annual Congress of the European Association of Nuclear Medicine, 19.-23.10.2013, Lyon, France
  • Abstract in refereed journal
    European Journal of Nuclear Medicine and Molecular Imaging 40(2013)2, S318

Permalink: https://www.hzdr.de/publications/Publ-18657
Publ.-Id: 18657


Synthesis and Evaluation of Novel 18F-Labeled Spirocyclic Piperidine Derivatives as σ1 Receptor Ligands for Positron Emission Tomography Imaging

Li, Y.; Wang, X.; Zhang, J.; Deuther-Conrad, W.; Xie, F.; Zhang, X.; Liu, J.; Qiao, J.; Cui, M.; Steinbach, J.; Brust, P.; Liu, B.; Jia, H.

A series of spirocyclic piperidine derivatives were designed and synthesized as σ1 receptor ligands. In vitro competition binding assays showed that 1'-(4-(2-fluoroethoxy)benzyl)-3H-spiro[2-benzofuran-1,4'-piperidine] (19) possessed high σ1 receptor affinity (Ki= 0.79 nM) and excellent σ12 subtype selectivity (350-fold) as well as high σ1/VAChT selectivity (799-fold). The radiolabeled compound [18F]19 was synthesized by substitution of the tosylate precursor 24 with [18F]fluoride, with isolated radiochemical yield of 35–60%, radiochemical purity of >99%, and specific activity of 30–55 GBq/Qmol. Biodistribution studies in ICR mice indicated that [18F]19 displayed excellent initial brain uptake and slow washout. Ex vivo autoradiography in Sprague-Dawley rat demonstrated high accumulation of the radiotracer in brain areas known to express high levels of σ1 receptors. MicroPET imaging and blocking studies confirmed the specific binding of [18F]19 to σ1 receptors in vivo.

Keywords: σ1 receptor; brain; spirocyclic piperidine derivatives; 18F; PET imaging

Permalink: https://www.hzdr.de/publications/Publ-18655
Publ.-Id: 18655


Phantom-based evaluation of quantification accuracy of combined PET/MRI

Langner, J.; Schramm, G.; Hofheinz, F.; Lougovski, A.; Steinbach, J.; van den Hoff, J.

Ziel/Aim:

A widely discussed question in PET is the quantitative accuracy (QA) of combined PET/MRI systems. To evaluate QA of the Philips Ingenuity TF PET/MR system we have performed phantom-based evaluations and compared them to measurements on traditional PET systems.

Methodik/Methods:

With the Philips PET/MR a SUV calibration is the standard procedure to calibrate the PET against a dose calibrator (DC). A dynamic scan is started at high activity (≈500 MBq) and run for 7 half-life times. Than a SUV validation with lower activity (≈70 MBq) is run as a static scan for 3 min. We augmented the validation protocol to start at higher activity and to run as a dynamic protocol. To evaluate the clinical relevant QA we have determined typical singles rates (SR) for whole-body (WB) scans. To analyse the influence of the MR-based attenuation (MRAC) we have created an attenuation template (AT) of the phantom and applied it.

Ergebnisse/Results:

The PET-derived activity concentrations and SUVs are significantly lower than calculated from the DC. Using the standard procedure the PET vs. DC ratio is 0.895=10.5% deviation at a level of 73.7 MBq (SR: 14.7 Mcps). For activity increasing from 8.6 to 89.7 MBq the PET/DC ratio decreases from 0.943 to 0.877, corresponding to deviations of 6–12% (SR: 3.8–17.0 Mcps). The use of an AT changes the deviation < 1%. For typical WB scans the SR were found to range from 8.0–16.6 Mcps, corresponding to a underestimates of true activity by 6.8–9.9%.

Schlussfolgerungen/Conclusions:

Our preliminary results show, that QA of the Philips PET/MR in phantoms is off by 6–12%. The effect shows a notable dead-time dependency and cannot be explained by inaccurate MRAC. In addition to the dead-time related variance of ≈3% there remains a systematic error in the calibration, which biases QA of clinical scans by ≈6%. Philips has been informed about the inconsistencies and has acknowledged to provide a fix.

  • Poster
    51. Jahrestagung der Deutschen Gesellschaft für Nuklearmedizin (DGN), 17.-20.04.2013, Bremen, Deutschland
  • Abstract in refereed journal
    Nuklearmedizin 52(2013), A77
    ISSN: 0029-5566

Permalink: https://www.hzdr.de/publications/Publ-18654
Publ.-Id: 18654


In-vivo evaluation of quantification accuracy of combined PET/MRI

Langner, J.; Schramm, G.; Hofheinz, F.; Lougovski, A.; Beuthien-Baumann, B.; Platzek, I.; Kotzerke, J.; Steinbach, J.; van den Hoff, J.

Ziel/Aim:

Quantitative accuracy (QA) of PET parameters like standardised uptake values (SUV) and tracer kinetic rate constants strongly depends on applicability of the (phantom-based) scanner calibration in-vivo. In a previous study we introduced a method for direct in-vivo QA evaluation: for 3 PET(/CT) systems the activity concentrations (Cs) of urine samples measured in a well-counter were compared to the Cs of PET images of the bladder in 56 patients. That study showed a small (7-12%) but systematic underestimation of the true Cs by PET. To address the widely discussed question of QA of combined PET/MRI we have applied this method to our Philips PET/MR.

Methodik/Methods:

Up to now 10 clinical F18-FDG scans have been evaluated. The bladder region was imaged as the last bed position and urine samples collected afterwards. Using the ROVER software, 3D region-of-interests (ROI) of the bladder were delineated by 3 observers. To exclude partial volume effects ROIs were concentrically shrunk by 8–10 mm. Then, Cs were determined in the PET images of the bladder as well as in the urine samples using a cross-calibrated well-counter.

Ergebnisse/Results:

The measured Cs and SUVs are significantly lower in PET/MR than in the well-counter: ratio=0.773±0.035 (mean±SEM) [0.617–0.942] (p=0.00011). After correcting for known (but not yet fixed) inconsistencies in the manufacturer’s scanner calibration of the Philips PET/MR, the ratio is 0.827±0.035 [0.664–1.004] (p=0.0011).

Schlussfolgerungen/Conclusions:

Our preliminary results indicate that the Philips PET/MR underestimates true Cs by ≈17% in-vivo which is ≈7% larger than we observed for PET(/CT). The requirement to apply a correction factor due to inconsistencies in the manufacturer’s provided calibration and similar deviations reported on other PET/MR systems show that vendors of PET/MR systems need to pay special attention regarding QA. In this context, our method might serve as a convenient method to evaluate the actual QA in-vivo.

  • Lecture (Conference)
    51. Jahrestagung der Deutschen Gesellschaft für Nuklearmedizin (DGN), 17.-20.04.2013, Bremen, Deutschland
  • Abstract in refereed journal
    Nuklearmedizin 52(2013), A50
    ISSN: 0029-5566

Permalink: https://www.hzdr.de/publications/Publ-18653
Publ.-Id: 18653


Preclinical radiopharmacological characterization of a Cu-64-labeled bis(2-pyridylmethyl) )-1,4,7-triazacyclononane bombesin analogue

Bergmann, R.; Ruffani, A.; Graham, B.; Spiccia, L.; Steinbach, J.; Pietzsch, J.; Stephan, H.

Ziel/Aim:

The bifunctional chelating agent 2-[4,7-bis(2-pyridylmethyl)-1,4,7-triazacyclononan-1-yl]acetic acid (DMPTACN-COOH) has been coupled to the stabilized bombesin (BBN) derivative [Cha13,Nle14]-BBN(7–14) using the spacer homo-Glu-Ala-Ala, was radiolabeled with the positron emitter copper-64, and the new radiotracer was preclinically characterized.

Methodik/Methods:

The in vitro and in vivo binding characteristics of the Cu-64-labeled bombesin conjugate in gastrin-releasing peptide receptor (GRPR) over-expressing prostate cancer (PC-3) cells/tumors have been evaluated. Biodistribution and metabolism studies were performed in Wistar rats. Small animal PET imaging was carried out to evaluate the biokinetics and tumor accumulation in tumor bearing NMRI nu/nu mice.

Ergebnisse/Results:

The pendant carboxylic group enables this derivative to be conjugated to the N-terminal amino acid residues of the peptide. The resulting radiocopper(II)-ligand complex exhibits high stability. The IC50 value on PC3 cells was 15 nM, the specific binding was confirmed by high uptake in the GRPR-rich pancreas used as reference organ. The peptide showed a good metabolic stability, however, it was fast eliminated by the kidneys. The PC3 tumors in the mice could be clearly imaged with tumor-to-muscle ratios steadily increasing over the time up to 30. The tumor uptake could be blocked by GRP.

Schlussfolgerungen/Conclusions:

Preclinical characterization of the Cu-64-labeled DMPTACN-COOH with incorporation of a single glutamic acid residue within the spacer between bombesin and the radiolabeled complex showed that the probe represents a promising GRPR radiotracer.

  • Lecture (Conference)
    51. Jahrestagung der Deutschen Gesellschaft für Nuklearmedizin (DGN), 17.-20.04.2013, Bremen, Deutschland
  • Abstract in refereed journal
    Nuklearmedizin 52(2013), A36-A37
    ISSN: 0029-5566

Permalink: https://www.hzdr.de/publications/Publ-18652
Publ.-Id: 18652


Comparison of current reconstruction algorithms for F18-FDG-PET based volume definition – phantom measurements

Rogasch, J.; Hofheinz, F.; Furth, C.; Ruf, J.; Grosser, O.; Mohnike, K.; Hass, P.; Amthauer, H.; Steffen, I. G.

Ziel/Aim:

Oncological microtherapy planning, e.g. brachytherapy, based on PET-datasets requires exact quantification and volume definition. The aim of this study was to analyze the influence of current reconstruction algorithms on SUVmax, metabolic volumes and spatial resolution using phantom measurements.

Methodik/Methods:

Measurements were performed on a SIEMENS Biograph mCT 64 using a cylindrical phantom (volume, 6595 ml) containing 4 spheres (14-177 ml) filled with F18-FDG (50 kBq/ml) resulting in 3 background fractions (BGF). Images were reconstructed applying 5 algorithms (3D-OSEM, FBP, FBP-TOF, HD-PET, ultraHD-PET) and two slice thicknesses (3 mm, 5 mm). Segmentation of sphere volumes was performed using semiautomatic tumor-to-background algorithm (ROVER). Spatial resolution was determined using point spread function and fitting of radial activity profiles.

Ergebnisse/Results:

The highest SUVmax deviations were found between ultraHD-PET and FBP-TOF with a mean absolute difference of 1.3 (range, 0.7–2.1) and a corresponding mean relative difference of 13.2% (range, 8.2–20.9%). Metabolic volume difference to reference volume was significantly associated to reconstruction algorithm (p<0.05), background fraction (BGF3 vs BGF1, p<0.001; BGF2 vs BGF1, p=0.1), sphere diameter (p<0.001) but not to slice thickness (p=0.3). Best spatial resolution for BGF1 and BGF2 was detected for ultraHD-PET (5.3/4.5 mm) compared to FBP (6.8/6.6 mm) and 3D-OSEM (5.9/5.4). In contrast, similar spatial resolutions were detected for BGF3 ranging from 5.9 mm (3D-OSEM/FBP) to 6.5 mm (HD-PET). However, TrueX-algorithms (HD-PET, ultraHD-PET) showed substantial edge elevations in radial activity profiles (Gibbs artifacts).

Schlussfolgerungen/Conclusions:

Reconstruction algorithms showed substantial effect on SUVmax. This might be of clinical importance if PET quantification is used in oncological microtherapy planning. The clinical impact of high spatial resolution combined with Gibbs artifacts in TrueX reconstructions has to be analyzed in further trials.

  • Lecture (Conference)
    51. Jahrestagung der Deutschen Gesellschaft für Nuklearmedizin (DGN), 17.-20.04.2013, Bremen, Deutschland
  • Abstract in refereed journal
    Nuklearmedizin 52(2013), A26
    ISSN: 0029-5566

Permalink: https://www.hzdr.de/publications/Publ-18651
Publ.-Id: 18651


Population averaged image derived arterial input function in 15-O Water PET

Hofheinz, F.; Langner, J.; Beuthien-Baumann, B.; Steffen, I. G.; Apostolova, I.; Burchert, R.; Steinbach, J.; Kotzerke, J.; van den Hoff, J.

Ziel/Aim:

Arterial input function (IF) determination is traditionally based on arterial blood sampling which is invasive and ill-suited for clinical routine. Alternatively, one can use a population averaged IF determined via blood samples (BSIF) in a separate study. We present a strategy for generation of a population averaged image derived IF (IDIF) in brain investigations.

Methodik/Methods:

An image subvolume enclosing the carotid arteries is manually defined. Further processing is fully automated: 1: peak phase detection of the IF, 2: threshold based, background aware delineation using peak phase optimized for small structure size (~ 5 mm), 3: time activity curve generation, 4: model free recovery coefficient (R) determination 5: recovery and spillover correction according to Cm = R x Ct + (1 - R) x B, Cm/Ct: measured/true signal/IF, B: local background. This method was applied to 48 15-O Water brain studies (acquired with an ECAT HR+ PET). The resulting IFs were averaged, leading to a population averaged image derived IF (IDIF). Gray matter perfusion was computed from the Kety-Schmidt model assuming a partition coefficient in gray matter of 0.9 (f1). Perfusion was also computed using a BSIF from a different institution (f2). f1 and f2 were compared.

Ergebnisse/Results:

f1 and f2 are strongly correlated (Pearson 0.999) and differences are small: (f2-f1)/f2 = (9.7 +/- 0.9)% (mean +/- sd), range 6.7% - 12.7%.

Schlussfolgerungen/Conclusions:

The presented method allows to generate an IDIF which reproduces the results achieved with BSIF with good accuracy. One significant advantage of the new approach is the ease of regeneration of the IDIF for each study group (e.g. after injection and acquisition protocol changes). Due to statistical fluctuations of vessel delineation individual IF determination is not yet possible with this method due to the modest reconstructed resolution of the HR+ data. This might become possible when using state-of-the-art scanners and reconstruction algorithms.

  • Lecture (Conference)
    51. Jahrestagung der Deutschen Gesellschaft für Nuklearmedizin (DGN), 17.-20.04.2013, Bremen, Deutschland
  • Abstract in refereed journal
    Nuklearmedizin 52(2013), A21
    ISSN: 0029-5566
  • Poster
    Annual Congress of the European Association of Nuclear Medicine, 19.-23.10.2013, Lyon, France
  • Abstract in refereed journal
    European Journal of Nuclear Medicine and Molecular Imaging 40(2013), S302-S303
    ISSN: 1619-7070

Permalink: https://www.hzdr.de/publications/Publ-18650
Publ.-Id: 18650


Relative cerebrovascular reserve capacity in Moyamoya disease assessed by brain perfusion imaging: PET versus SPECT in the same patients

Steffen, I. G.; Apostolova, I.; Michel, R.; Schulze, O.; Rosner, C.; Hofheinz, F.; Prasad, V.; Brenner, W.; Vajkoczy, P.; Buchert, R.

Ziel/Aim:

Moyamoya disease (MMD) is characterized by progressive stenosis or occlusion of the terminal internal carotid arteries with varying development of collaterals requiring the exact characterization of hemodynamics for adequate therapy. The aim of the present study was to compare perfusion SPECT and PET with O-15-water in the same patients.

Methodik/Methods:

Static SPECT and dynamic PET were performed within 1-5 d in 9 MMD patients (18-67 y), both in resting state and after vasodilatory challenge with acetazolamide. The PET data were analyzed with the Watabe reference tissue method for the voxelwise computation of the regional cerebral blood flow. Vasodilatation and resting images were coregistered, stereotactically normalized (SPM8) and smoothed (3d isotropic Gaussian kernel, 20 mm FWHM). The relative cerebrovascular reserve (rCVR) was computed voxel-by-voxel according to the formula rCVR = 100*(s*vasodilatation – resting)/resting. The scale factor (s) was determined to a mean rCVR of 50%. The resulting rCVR maps were assessed visually and using standard ROIS for ACA, MCA and PCA territory (left/ right). A general linear model was used to analyze the effect of modality (SPECT, PET) and territory (ACA, MCA, PCA) on rCVR.

Ergebnisse/Results:

The pattern of rCVR differed significantly between SPECT and PET in 5/9 patients according to visual inspection. PET showed additional or more extended regions with reduced rCVR in these cases. The ROI analysis revealed a significant effect of the modality (p=0.015) and a highly significant modality*territory interaction (p=0.000). PET-rCVR was lower than SPECT-rCVR in the ACA and MCA territory, whereas it was higher in the PCA territory.

Schlussfolgerungen/Conclusions:

There was a substantial difference in the cerebrovascular reserve capacity as measured by SPECT versus PET, both visually and quantitatively. The modality*territory interaction suggests that PET is more accurate than SPECT, as MMD often spares the posterior circulation. However, this has to be confirmed in further studies.

  • Lecture (Conference)
    51. Jahrestagung der Deutschen Gesellschaft für Nuklearmedizin (DGN), 17.-20.04.2013, Bremen, Deutschland
  • Abstract in refereed journal
    Nuklearmedizin 52(2013), A14
    ISSN: 0029-5566

Permalink: https://www.hzdr.de/publications/Publ-18649
Publ.-Id: 18649


Kupfer-64 markierte Peptid-Konjugate an epidermalen Wachstumsfaktor-Rezeptor (EGFR)-exprimierenden Zellen

Sihver, W.; Starke, F.; Heldt, J.-M.; Sachse, S.; Naumann, S.; Pietzsch, H.-J.; Steinbach, J.

Ziel/Aim:

Der EGFR wird oft überexprimiert in verschiedenen Tumorarten. Daher werden geeignete radionuklidmarkierte EGFR-Liganden für eine gezielte Tumordiagnostik mittels bildgebender Verfahren, z. B. PET, entwickelt. Zwei kürzlich beschriebene EGFR-spezifische Peptide GE11 (1) und D4 (2) sollten mit Chelatoren sowie Spacern so konjugiert werden, dass sie mit dem PET-Nuklid Kupfer-64 markiert werden können. Mit einem der markierten Peptid-Konjugate sollte das Bindungsverhalten (Zeitabhängigkeit und Affinität) an Zellmembranen charakterisiert werden.

Methodik/Methods:

Die Peptide wurden am N-Terminus jeweils mit verschiedenen Spacern sowie mit dem Chelator NOTA verknüpft und anschließend mit Kupfer-64 radiomarkiert. Für Bindunggsassays wurden Membranen der EGFR-exprimierenden A431-Zellen (epidermoides Karzinom) und FaDu-Zellen (Plattenepithelkarzinom) untersucht. Kinetik- und Sättigungs-Assays wurden mit einem Kupfer-64 markierten NOTA-D4-Konjugat ([64Cu]Cu-D4-JM) durchgeführt.

Ergebnisse/Results:

Die Peptidkonjugate konnten mit einer Ausbeute von 75-91% hergestellt werden. Bei der Radiomarkierung mit Kupfer-64 konnten spezifische Aktivitäten von bis zu 1000 GBq/µmol erreicht werden, jedoch wurden diese für Bindungsassays auf etwa 30 GBq/µmol eingestellt. Für die Bindung mit [64Cu]Cu-D4-JM an A431-Membranen war nach 1 Stunde Assoziation das Bindungsgleichgewicht erreicht, an FaDu-Membranen nach 2 Stunden nicht vollständig. TDiss½ lag unter 5 min. Die Affinität mittels Sättigung ergab für A431- und für FaDu-Membranen Kd-Werte von 19 bzw. 42 nM.

Schlussfolgerungen/Conclusions:

Mit GE11 und D4 konnten verschiedene EGFR-spezifische Peptid-Konjugate erfolgreich hergestellt werden. Nachdem [64Cu]Cu-D4-JM an Zellmembranen untersucht wurde, sind weiterführende Assays an intakten Zellen sowie Tumoraufnahme an Xenograft tragenden Mäusen geplant.

Literatur/References:

(1) Li Z, Zhao R, Wu X et al. FASEB J. 2005, 19(14), 1978-85
(2) Song S, Liu D, Peng JL, et al. Intl. Conf. on Biomedical and Pharmaceutical Engineering 2006, 290-3

  • Lecture (Conference)
    51. Jahrestagung der Deutschen Gesellschaft für Nuklearmedizin (DGN), 17.-20.04.2013, Bremen, Deutschland
  • Abstract in refereed journal
    Nuklearmedizin 52(2013), A12
    ISSN: 0029-5566

Permalink: https://www.hzdr.de/publications/Publ-18648
Publ.-Id: 18648


Fluor-18-markierte Telopeptidderivate als Substrat-basierte Radiotracer zur Bildgebung der Lysyloxidase in vivo

Kuchar, M.; Wodtke, R.; Bergmann, R.; Lenk, J.; Mosch, B.; Pietzsch, J.; Löser, R.

Ziel/Aim:

Dem Enzym Lysyloxidase (LOX, EC 1.4.3.13), wird eine Schlüsselfunktion für die Hypoxie-induzierte Tumormetastasierung zugeschrieben (1). Ziel unserer Untersuchungen war die Entwicklung Fluor-18-basierter Radiotracer, die eine In-vivo-Bildgebung dieses Enzyms ermöglichen.

Methodik/Methods:

Das N-terminale Telopeptid der α1-Kette des Typ-I-Kollagens und davon abgeleitete Peptide, die potentielle LOX-Substrate sind, wurden an von den funktionellen Lysinresten verschiedenen Aminogruppen Fluor-18-markiert. Dazu wurde eine Methode entwickelt, die die selektive F-18-Fluorobenzoylierung von Peptiden mit [F-18]SFB ermöglicht (2). Die metabolische Stabilität und Bioverteilung der Radiotracer wurde in normalen männlichen Wistarratten untersucht. Über die Wechselwirkung der verschiedenen Lysin-enthaltenden Peptide mit Atelokollagen wurde durch Oberflächenplasmonenresonanz (SPR) Aufschluss erhalten. Verschiedene Tumorzelllinien wurden in vitro auf die Expression der Lysyloxidase hin untersucht. Die Charakterisierung der Verbindungen erfolgte an A375-Tumormäusen durch dynamisches Kleintier-PET-Imaging und Ex-vivo-Autoradiographie.

Ergebnisse/Results:

Die F-18-fluorbenzoylierten Telopeptidderivate wurden in hohen radiochemischen Ausbeuten und Reinheiten synthetisiert. Alle Peptide zeigten eine gute In-vivo-Stabilität, insbesondere ein cyclisches Derivat des N-Telopeptids. In den Bioverteilungsstudien konnten keine Organanreicherung und eine schnelle renale Eliminierung beobachtet werden. Die Telopeptid-Kollagen-Interaktion konnte erstmals quantitativ untersucht werden.

Schlussfolgerungen/Conclusions:

Geeignete LOX-Substrate wurden Fluor-18-markiert und in vivo eingehend charakterisiert. Trotz ungünstiger Pharmakokinetik infolge schneller renaler Eliminierung zeigen die Tracer das Potential, die LOX-Aktivität in vivo abzubilden.

Literatur/References:

(1) J. T. Erler, K. L. Bennewith, M. Nicolau et al. Nature 2006, 440, 1222-1226
(2) M. Kuchar, M. Pretze, T. Kniess et al. Amino Acids 2012, 43, 1431-1443

  • Lecture (Conference)
    51. Jahrestagung der Deutschen Gesellschaft für Nuklearmedizin (DGN), 17.-20.04.2013, Bremen, Deutschland
  • Abstract in refereed journal
    Nuklearmedizin 52(2013), A11
    ISSN: 0029-5566

Permalink: https://www.hzdr.de/publications/Publ-18647
Publ.-Id: 18647


Automatisierte F-18-Fluorethylierung als Markierungsmethode neuer potentieller COX-2 Inhibitoren

Laube, M.; Kniess, T.; Pietzsch, J.; Steinbach, J.

Ziel/Aim:

Das Enzym Cyclooxygenase-2 reguliert entzündungsassoziierte Prozesse und wird in vielen Tumoren exprimiert. Die Visualisierung der COX-2 Expression in vivo durch PET könnte daher neue Ansatzpunkte zur Charakterisierung von Tumoren liefern. Um erstmals zu F-18-Fluorethoxy-substituierten COX-2 Inhibitoren zu gelangen und um unterschiedliche COX-2 Inhibitoren mit mono- und bizyklischer Kernstruktur als PET-Tracer zur Verfügung zu stellen, entwickelten wir eine universelle, automatisierte Markierungsmethode.

Methodik/Methods:

Die Entwicklung zweier neuer Fluorethoxy-substituierter Derivate 2-(4-(2-Fluorethoxy)phenyl)-3-(4-(methansulfonyl)phenyl)pyrazolo[1,5-b]pyridazine (A) und 1-(2-Fluorethoxy)-4-(2-(4-(methansulfonyl)phenyl)cyclopent-1-enyl)benzen (B) erfolgte ausgehend von den Ethoxy- bzw. Methoxy-substituierten Derivaten A* und B* (IC50 COX-2: 3 bzw. 5 nM) (1,2). F-18-A und F-18-B wurden in einer automatisierten Syntheseapparatur (TracerlabFX-N) unter optimierten Parametern durch indirekte Markierung der entsprechenden Hydroxyl-Präkursoren mit 1,2-[F-18]Fluorethyltosylat (F-18-C) hergestellt.

Ergebnisse/Results:

Durch enzymatischen Assay wurde für A und B bestätigt, daß die Fluorethylgruppe die COX-2 Inhibitoraktivität nur wenig beeinflusst. Mittels zwei-Stufen/ein-Topf-Synthese inklusive HPLC Reinigung konnte F-18-A ausgehend von [F-18]Fluorid in 70 min mit 7,5% RCA (n=5; zerf.korr.) hergestellt werden (RCR >95%; spezif. Aktivität 27-71 GBq/µmol). In analoger Weise wurde F-18-B in 80 min mit 7,8% RCA (n=7; zerf.korr.) erhalten (RCR 98%; spezif. Aktivität 19-43 GBq/µmol).

Schlussfolgerungen/Conclusions:

Durch die entwickelte automatisierte F-18-Fluorethylierung konnten die COX-2 Inhibitoren F-18-A und F-18-B erfolgreich hergestellt werden, ihre radiopharmakologische Evaluierung findet zur Zeit statt. Die Methode bietet einen effektiven Zugang zur Radiomarkierung von COX-2 Inhibitoren mit Methoxy- bzw. Ethoxy-Funktionen.

Literatur/References:

(1) Beswick et al., Bioorg. Med. Chem. Lett. 2004, 14, 5445.
(2) Wüst et al., Bioorg. Med. Chem. 2008, 16, 7662.

  • Lecture (Conference)
    51. Jahrestagung der Deutschen Gesellschaft für Nuklearmedizin (DGN), 17.-20.04.2013, Bremen, Deutschland
  • Abstract in refereed journal
    Nuklearmedizin 52(2013), A11
    ISSN: 0029-5566

Permalink: https://www.hzdr.de/publications/Publ-18646
Publ.-Id: 18646


Truncation artifacts in hybrid PET/MR - evaluation and compensation

Schramm, G.; Langner, J.; Hofheinz, F.; Petr, J.; Beuthien-Baumann, B.; Platzek, I.; Kotzerke, J.; Steinbach, J.; van den Hoff, J.

Ziel/Aim:

MR-based attenuation correction in hybrid PET/MR imaging is affected by the reduced transaxial FOV of the MR (40cm) in comparison to that of the PET scanner (60cm) which leads to truncation artifacts in the MR-based attenuation map
(MRMap). In this study we investigate the quantitative influence of truncation artifacts on the reconstructed whole-body PET image volumes and present a new method for truncation compensation (TC).

Methodik/Methods:

Data sets of 17 whole-body FDG patients (BMI 16-38) examined with an Philips Ingenuity PET/MR with arms down were reconstructed using different techniques for TC: (1) no TC (PET-noTC), (2) vendor-provided TC (PET-TC1), (3) newly
developed TC (PET-TC2) based on automatic 3D segmentation of PET-noTC. In all PET volumes, the resulting SUVmax/mean of ROIs in different body regions (e.g. heart, bladder, mediastinum, kidneys, arms etc.) were compared.
Furthermore, a correlation analysis between all voxels in the trunk and truncated arms was performed.

Ergebnisse/Results:

Residual artifacts in the truncation compensated MRMaps were found in 11 (TC1)and 3 (TC2) out of 17 cases. Average SUVmax differences between PET-noTC and PET-TC1/PET-TC2 were: -2.5%/-3.2% (bladder), -4%/-3.4% (kidney),
-3.2%/-3.5% (heart), -2.8/-3.3% (abdomen), -29%/-37% (arms). The correlation analysis showed average SUV deviations of -5% to -1% and -60% to -30% depending on patients' BMI for all voxels in the trunk and truncated arms, respectively.

Schlussfolgerungen/Conclusions:

In whole-body PET imaging, truncation of the arms in the MRMap leads to an average SUV underestimation of ca. 3% in the trunk. In the truncated areas SUV underestimations in the range of 30-60% can be expected. Truncation
compensation based on PET-noTC is straightforward and improves quantification accuracy distinctly. According to our experience the procedure is also well suited for clinical routine.

  • Lecture (Conference)
    51. Jahrestagung der Deutschen Gesellschaft für Nuklearmedizin (DGN), 17.-20.04.2013, Bremen, Deutschland
  • Abstract in refereed journal
    Nuklearmedizin 52(2013), A6
    ISSN: 0029-5566

Permalink: https://www.hzdr.de/publications/Publ-18645
Publ.-Id: 18645


Environmental parameters that determine distribution coefficients of radionuclides for repositories

Stockmann, M.; Brendler, V.; Richter, C.; Flügge, J.; Britz, S.; Noseck, U.

In order to treat radionuclide sorption processes in natural systems more realistically, temporally and spatially variable distribution coefficients (smart Kd values) are calculated as a function of important environmental parameters such as pH, ionic strength (IS), concentration of dissolved inorganic carbon [DIC], calcium [Ca] and radionuclides [RN]. This smart Kd concept is implemented into the transport code r³t [1].
As a test of the modified code r³t and sensitivity analysis of radionuclide sorption regarding the mentioned environmental parameters, a possible future climate transition (seawater transgression) at Gorleben site / Germany was modelled [2]. Seawater inundation drastically influences the distribution and values of all environmental parameters. Chemical changes cause dissolution or precipitation of calcite and these in turn affect the pH, DIC and Ca concentration. In consequence the Kd values and therewith the transport of radionuclides is impacted.
The results of the calculations are plausible: environ-mental parameters follow expected trends and major dependencies. As a consequence of the low Ca and DIC concentration in seawater, calcite dissolves in the aquifer and causes an increase of the pH. The Kd values change according to the changes in environmental parameters. The pH has the most dominant impact on the smart Kd values for most of the considered RNs, except for Pu and Th, for which the DIC concentration has the strongest impact. Under the assessed conditions for seawater transgressions the smart Kd values of Cs, Ni, Am and Np(V) increase, those of Se(VI) and U(VI) decrease with increasing pH. The smart Kd value particularly of Pu and Th decreases with increasing DIC concentration.

  • Poster
    Goldschmidt 2013, 25.-30.08.2013, Florence, Italy

Permalink: https://www.hzdr.de/publications/Publ-18644
Publ.-Id: 18644


Microorganisms in saline environments

Geissler, A.; Bachvarova, V.; Flemming, K.; Selenska-Pobell, S.

The long-term safety of nuclear waste in deep geological repositories is an important issue in the German society. The migration of actinides and long-lived fission products within the respective host rock and the transport behaviour after a possible release from the repository should be well known. Presence of microorganisms was shown in the subsurface geologic layers, including salt formations, which are considered as potential host rocks /1/. This is of interest because microbes can affect physical and geochemical conditions (e.g. pH, Eh, release of gases) on site and they can also interact with actinides. Important interaction processes are biosorption, bioaccumulation, biotransformation, biomineralization and microbial enhanced chemisorption /2/.
In this work microbial communities were investigated in two different saline environments - the Arava desert in Israel and the salt formation near Gorleben village in Germany.

DESCRIPTION OF THE WORK

Total DNA was recovered from the salt crust (7EY) and from 0 to 3cm depth (10EY) samples of the Arava desert and from one hydrocarbon rich sample C1 from the Gorleben site. Direct molecular analyses of prokaryotic communities were performed by using bacteria specific 16S rRNA gene primers 27F and 1513R /3/ and archaea specific 16S rRNA gene primers 21F and 968R /4/.
Modified R2A medium was used for cultivation of halophilic microbial isolates as described in /5/.

RESULTS

It was demonstrated that the archaeal communities in both 7EY and 10EY samples were predominated by Halobacteriaceae /4/. The recently actualized affiliation of the 16S rRNA gene sequences demonstrated presence of representatives of the genera Haloplanus, Natronomonas, Halobacterium and Halolamina. Several haloarchaeal isolates were cultivated from the salt crust sample 7EY and one of them was characterized as Halobacterium sp. UJ-EY-1 /5/.
On the bacterial phylum level, the samples 7EY and 10EY were predominated by Bacteroidetes, which were accompanied by Firmicutes, Gamma-, Alpha-, and Delta-proteobacteria occurring in a sample-specific way. In addition, differences were found on the species level.
Preliminary results demonstrate that Bacteroidetes are rather abundant in the Gorleben sample C1 where, in addition, Firmicutes are also predominant. Different Proteobacteria are identified in this sample as well. Further investigations of microbial diversity in this and other samples from the Gorleben site are in progress.

At this step of investigation characterization of microbial communities in salt formations representative for potential nuclear waste disposals is ongoing. The next step will be to understand the microbe-actinide interactions of the salt-specific microorganisms. This knowledge will be used to take the microbial activity into account in evaluating the long-term safety of the repositories hosted in salt formations.

REFERENCES

1. Vreeland, R.H., Pisseli A.F., McDonnough, S., Meyers, S. Distribution of halophilic bacteria in a subsurface salt formations. Extremophiles 2, 321-331 (1998).
2. Lloyd, J. R., Macaskie, L. E.: Biochemical basis of microbe-radionuclide interactions. Interactions of Microorganisms with Radionuclides, eds Keith-Roach, M. J., Livens, F. R. Elsevier Science Ltd., 313-342 (2002).
3. Geissler, A., Selenska-Pobell, S.: Addition of U(VI) to a uranium mining waste sample and resulting changes in the indigenous bacterial community. Geobiology 3, 275-285 (2005).
4. Buchvarova, V., Jankowski, U., Flemming, K., Selenska-Pobell S. Halophilic archaeal populations in Arava Desert (Israel) as examined by using direct molecular and cultivation methods FZR-Report 511, p. 34 (2009).
5. Jankowski, U., Flemming, K., Selenska-Pobell, S. Characterization of a Halobacterium sp. isolate cultivated from samples collected from Arava Desert. FZR-Report 511, p. 35 (2009).

Keywords: Microbial diversity; salt formations; radioactive waste depositories

  • Lecture (Conference)
    ABC-Salt Workshop III, 15.-17.04.2013, Santa Fe, New Mexico, USA

Permalink: https://www.hzdr.de/publications/Publ-18643
Publ.-Id: 18643


Vibrational spectroscopic study of Np(V) sorption on mineral oxides

Müller, K.; Berger, J.; Cordiez, M.; Gröschel, A.; Foerstendorf, H.

Mineral oxides play a decisive role in regulating the mobility of contaminants in the environment because of their widespread occurrence in rocks and soils, their tendency to form coatings on mineral surfaces and their wide-ranging technical applications [1].
Due to its long half-life and its toxicity, Np-237 is considered as a major contaminant of the ecosystem in the long-term safety assesment of nuclear waste repositories. The pentavalent state is environmentally most relevant [2].
For the first time, in-situ Np(V) sorption is comparatively studied on the oxyhydroxides of Fe, Mn, Si and Ti by ATR FT-IR spectroscopy under a variety of environmentally relevant sorption conditions. From the results, the formation of binary inner-sphere complexes on oxides of Si, Mn, Fe and Ti can be derived [3]. In case of ferrihydrite, the formation of an additional ternary Np-carbonato surface species is assumed. In addition, time resolved spectra provide kinetic information on the surface reactions.
[1] Dixon J. B. et al.(1989) Minerals in soil environments. Madison, Wisc.: Soil Science Soc. of America. 1244. [2] Kaszuba J. P. et al. (1999) Env. Sci. & Techn. 33(24), 4427-4433. [3] Müller K. et al. (2009) Env. Sci. & Techn. 43(20): p. 7665-7670

  • Lecture (Conference)
    Goldschmidt 2013, 25.-30.08.2013, Florence, Italy
  • Abstract in refereed journal
    Mineralogical Magazine 77(2013)5, 1806

Permalink: https://www.hzdr.de/publications/Publ-18642
Publ.-Id: 18642


Raman imaging of copper ores

Kostudis, S.; Hof, M.; Kutschke, S.; Pollmann, K.

In Middle Europe large deposits of Kupferschiefer involve the Upper Lusatia, the northeastern part of Saxony. The regional Kupferschiefer raised again interest of both industry and science because in this region its copper content constitutes the most important natural copper resource. There is no efficient biotechnological approach applied yet due to the fact that Kupferschiefer is complexly composed comprising different sulfidic minerals, carbonates and organic compounds. Bioleaching, which means the use of microorganisms and their metabolites to extract metals from their ores, reduces costs of high energy input and avoids the usage of toxic chemicals thus benefitting environment (Narayan 2009) and employees.
Raman spectroscopy enables a fast and specific chemical identification of minerals and ores (Hope 2001) as well as the detection of changes e.g. that are caused by oxidation (García-Meza 2012). Also Raman spectroscopic imaging of biotic components such as biofilms has already been performed (Virdis 2012).
We aim to use Raman spectroscopy to investigate the interactions of microorganisms and ore surface: Different polished sections of bornite, chalcopyrite (both from Henderson Mine, Namagualand, South Africa), chalcosite (Ashio, Japan) and copper shale (Polkovice, Poland) were analysed by polarising microscopy to ensure correct spectra assignment. Subsequently identical areas were analysed by Raman imaging using 2D scanning function. After incubation with microorganisms the sections will be investigated again in order to evaluate chemical changes of the ore surfaces, biofilm formation and to monitor bioleaching processes.

  • Poster
    RamanFest 2013 Symposium, 23.-24.05.2013, Lille (Nord), Frankreich

Permalink: https://www.hzdr.de/publications/Publ-18641
Publ.-Id: 18641


Identification of multiple S-layer genes that are expressed by Lysinibacillus sphaericus JG-B53 – a bacterial survival strategy in metalliferous environments?

Lederer, F.; Weinert, U.; Günther, T.; Raff, J.; Pollmann, K.

Generally, heavy metal contamination of the environment is a result of either natural events like volcanic emissions or human activities such as mining processes. High concentrations of heavy metals are toxic to the majority of organisms. However, several bacteria exhibit surprising strategies to survive in metalliferous environments. These strategies are attractive for novel bio-based resource technologies. Their understanding is the purpose of our research.
Aim of this study was the identification of bacterial methods to accept heavy metals in their environment. Genes that are related to the bacterial heavy metal tolerance strategy were analysed.
Lysinibacillus sphaericus JG-B53, an isolate from the uranium mining waste pile Haberland, was studied using genome sequencing analyses in order to identify strain intrinsic survival strategies like surface (S) layer proteins with metal specific binding affinities and metal specific transporter proteins. The genome of Lysinibacillus sphaericus JG-B53 was sequenced using the Next Generation Sequencing Technology. Bioinformatic analyses of generated data were performed with the Genomics Workbench (CLCbio). The expression of selected genes was studied using mRNA methods. Genes and encoded proteins were characterised with special analysing tools.
The genome of Lysinibacillus sphaericus JG-B53 encodes at least 13 S-layer like proteins and 3 metal ion exporter protein genes for metals that occur in the natural habitat. Their characteristics were analysed with multiple gene and protein analysing programs. Using cDNA analyses the expression of 6 putative S-layer proteins was detected.
Future studies will analyse recombinant S-layer proteins regarding their lattice symmetry and metal binding affinities.

  • Lecture (Conference)
    5th Congress of European Microbiologists - FEMS 2013, 21.-25.07.2013, Leipzig, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-18640
Publ.-Id: 18640


Milling Result Prediction

Matos Camacho, S.; Leißner, T.; Atanasova, P.; Kamptner, A.; Rudolph, M.; Peuker, U. A.; van den Boogaart, K. G.

Fine grained ore can only be exploited with finer milling, which results in additional milling costs. The ability to infer the optimal milling parameters and corresponding grades of recovery from microstructural information allows optimal extraction and predicting processing costs and final recovery. The MLA (Mineral Liberation Analyzer) allows quantifying the 2D size of grains in the ore. We have developed a method to predict the effect of milling from milling experiments and MLA-images to the 3D liberation of the value mineral in the ore.

Keywords: grinding; geometallurgy; MLA; milling

  • Lecture (Conference)
    15th Annual Conference of the International Association for Mathematical Geosciences - IAMG 2013, 02.-06.09.2013, Madrid, Espana
  • Contribution to proceedings
    15th Annual Conference of the International Association for Mathematical Geosciences - IAMG 2013, 02.-06.09.2013, Madrid, Espana
    Mathematics of Planet Earth - Proceedings of the 15th Annual Conference of the International Association for Mathematical Geosciences, Berlin, Heidelberg: Springer, 978-3-642-32407-9, 717-721
    DOI: 10.1007/978-3-642-32408-6

Permalink: https://www.hzdr.de/publications/Publ-18639
Publ.-Id: 18639


Dendrimers as Nb3+ ligands: effect of generation on the efficiency of the sensitized lanthanide emission

Pillai, Z. S.; Ceroni, P.; Kubeil, M.; Heldt, J.-M.; Stephan, H.; Bergamini, G.

We have designed two novel dendrimers with cyclam cores with appended poly(amido amine) (PAMAM) dendrons, decorated at the periphery with four and eight dansyl chromophores, respectively. The photophysical properties of the dendrimers and their Nd3+ complexes have been investigated. The energy-transfer efficiency to the lanthanide ions from these dendrimers has been studied as a function of the generation. It has been observed that an increase in the dendrimer generation as well as the number of amide units enhances the energy transfer to the lanthanide ion.

Permalink: https://www.hzdr.de/publications/Publ-18638
Publ.-Id: 18638


Herstellung und Reinigung von 64Cu am Leipziger Zyklotron Cyclone® 18/9

Mansel, A.; Franke, K.; Fischer, S.; Steinbach, J.

Die Abteilung „Reaktiver Transport“ der Forschungsstelle Leipzig beschäftigt sich mit dem Migrations-/Sorptionsverhalten von (Schad)stoffen in geologischen Formationen. In aktuellen Projekten werden partikuläre, kolloidale, gelöste und komplexierte, toxische und radiotoxische Stoffe in Batch- und Säulenstudien untersucht. Bei der eingesetzten Radiotracertechnik kommen kurzlebige Radionuklide zum Einsatz. Am Leipziger Zyklotron Cyclone® 18/9 neu implementiert ist die 64Cu-Herstellung durch Protonenbeschuss von isotopenangereichertem 64Ni via (64Ni(p,n)64Cu)[1]. Das Target wird durch elektrolytische Abscheidung von ca. 5 mg 64Ni auf Goldfolien hergestellt. Die Bestrahlung erfolgt bei einem Protonenstrom von 20 µA bei Strahlzeiten von bis zu 7 Stunden und einer Projektilenergie von ca. 12 MeV. Die chemische Aufarbeitung des bestrahlten Nickels erfolgt durch Ionenchromatographie mit AG1-X8 aus salzsaurer Lösung[2,3]. 64Cu wird mit einer radiochemischen Ausbeute von ca. 95 % erhalten. Das wertvolle Targetmaterial (isotopenangereichert auf 95 %) wird mit ~ 90 % Ausbeute wiedergewonnen. Das produzierte Radionuklid wurde erfolgreich zur Visualisierung von Fluidtransport in Geomaterialien mittels PET[4] sowie in der Calixarenkomplexierung[5] eingesetzt.

Literatur:

[1] F. Szelecsényi, G. Blessing, S. M. Qaim, 1993, Appl. Radiat. Isot. 44(3) 575-580.
[2] M. A. Avila-Rodriguez, J. A. Nye, R. J. Nickles, 2007, Appl. Radiat. Isot. 65(10) 1115-1120.
[3] S. Thieme, M. Walther, H.-J. Pietzsch, J. Henninger, S. Preusche, P. Mäding, J. Steinbach, 2012, Appl. Radiat. Isot. 70(4) 602-608.
[4] M. Stoll, Diplomarbeit, in Bearbeitung, Universität Mainz.
[5] M. Poetsch, Masterarbeit, 2012, Universität Leipzig.

  • Lecture (Conference)
    Wissenschaftsforum Chemie 2013 - Fachgruppe Nuklearchemie, 01.-04.09.2013, Darmstadt, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-18635
Publ.-Id: 18635


Generation of electron beams with superconducting photoinjectors

Teichert, J.; Arnold, A.; Büttig, H.; Justus, M.; Lehnert, U.; Lu, P.; Michel, P.; Murcek, P.; Schurig, R.; Vennekate, H.; Xiang, R.; Kamps, T.; Rudolph, J.; Kneisel, P.; Will, I.

The production of beams with low emittance as well as high average current is one of the key techniques for future electron accelerators and next generation light sources. The superconducting radio-frequency photo electron source (SRF gun) has the potential to fulfill the requirements for these new accelerators. The presentation will give an introduction and overview of this type of modern electron injector. The main issues such as niobium cavity design and fabrication, cryomodule, radio-frequency system, photocathodes, drive laser will be discussed. The status of the various R&D project for SRF guns will be presented, and a comparison to alternative high-current injector concepts like DC photo guns and low-frequency, normal-conducting RF guns will be given.

Keywords: superconducting RF; electron source accellerator; photoelectron injector; niobium cavity; photo cathode

Related publications

  • Invited lecture (Conferences)
    LA3NET 1st Topical Workshop on Laser Based Particle Sources, 20.-22.02.2013, Geneva, Switzerland

Permalink: https://www.hzdr.de/publications/Publ-18634
Publ.-Id: 18634


Evidences for a more restricted Icelandic Ice cap re-advance after the Bølling warming period

Meriaux, A.-S.; Delunel, R.; Merchel, S.; Finkel, R.

Moraines dated north of Vatnajökull by cosmogenic surface exposure dating show that the Icelandic Ice cap (IIS) was less extended during the Younger Dryas than previously suggested. The data imply that this glacial advance was more complex and restricted in some glacial valleys in NE Iceland. While the IIS margins are relatively well constrained offshore by marine or coastal evidences, little is known about their onshore characteristics and rates of recession during the warmer Holocene periods. This is especially the case in the NE of Iceland where volcanic activity and major outburst floods (jökulhlaups) have removed a large amount of morphological evidences of past ice margins. Our study aimed at filling this chronological gap of the IIS inland during the late Quaternary deglaciation by dating past preserved ice margins using 36Cl and 3He cosmogenic nuclides.
We studied moraines and outwash located 44 km, 48 km and 60 km north of Vatnajökull, between the Jökulsà à Fjöllum and Jökulsà à Brú, the main northern glacial river systems draining the icecap. Preliminary 36Cl ages of the northernmost moraine at Skessugarður, 60 km north of present-day IIS and 65 km away from the coastline, indicate that the minimum exposure ages derived from Ca-rich plagioclases range from 11.0 + 1.2 ka to 13.4 + 1.4 ka with an average at 12.2 + 1.0 ka (+1 sigma, n=6), using the local Icelandic production rates for Ca spallation of Licciardi et al. (2008). These ages are close to the Younger Dryas at a time when the Icelandic Ice Sheet is thought to have re-advanced further north toward the coastline. Overall, our results call for a Revision of our understanding of the IIS deglaciation history and provide new tie-points for the calibration of the IIS models.
References: Licciardi et al., EPSL 267 (2008) 365–377.

Keywords: cosmogenic nuclide; AMS; deglaciation; iceland

Related publications

  • Poster
    EGU General Assembly 2013, 07.-12.04.2013, Wien, Österreich

Permalink: https://www.hzdr.de/publications/Publ-18633
Publ.-Id: 18633


Selenium(IV) Uptake by Maghemite (gamma-Fe2O3)

Jordan, N.; Ritter, A.; Scheinost, A. C.; Weiß, S.; Schild, D.; Hübner, R.

The mechanism of selenium(IV) uptake by maghemite was investigated on both the macroscopic and the molecular level. Maghemite nanoparticles exhibited fast adsorption kinetics toward selenium(IV). Batch experiments showed a decreased sorption with increasing pH (3.5-11).
Ionic strength variations (0.01 to 0.1 M NaCl) had no significant influence on selenium(IV) uptake. Electrophoretic mobility measurements revealed a significant shift toward lower values of the isoelectric point of maghemite upon selenium(IV) uptake, suggesting the formation of inner-sphere surface complexes. At the molecular level, using X-ray Absorption Fine-Structure Spectroscopy (EXAFS), the formation of both bidentate binuclear corner-sharing (C-2) and bidentate mononuclear edge-sharing (E-1) inner-sphere surface complexes was observed, with a trend toward solely E-1 complexes at high pH. The absence of a tridentate surface complex as observed for arsenic(III) and antimonite(III) might be due to the relatively small size of the (SeO3)-O-IV unit. These new spectroscopic results can be implemented in reactive transport models to improve the prediction of selenium migration behavior in the environment as well as its monitoring through its interaction with maghemite or maghemite layers at the surface of magnetite. Due to its chemical stability even at low pH and its magnetization properties allowing magnetic separation, maghemite is a promising sorbing phase for the treatment of Se polluted waters.

Keywords: selenium(IV); uptake; maghemite; EXAFS

Related publications

Permalink: https://www.hzdr.de/publications/Publ-18632
Publ.-Id: 18632


Efficient laser-driven proton acceleration in the ultra-short pulse regime

Zeil, K.; Bock, S.; Burris-Mog, T.; Bussmann, M.; Helbig, U.; Kluge, T.; Kraft, S. D.; Metzkes, J.; Debus, A.; Roeser, F.; Cowan, T. E.; Sauerbrey, R.; Schramm, U.; Beyreuther, E.; Karsch, L.; Laschinsky, L.; Naumburger, D.; Oppelt, M.; Richter, C.; Schürer, M.; Baumann, M.; Enghardt, W.; Pawelke, J.

Erläuterung des Prinzips der Laserprotonenbeschleunigung und Präsentation der Experimente des TNSA Beschleunigungsmechanismus unter Verwendung ultrakurzer Laserpusle. Weiterhin wird die Anwendung der erzeugten Protonenpulse für strahlenbioloigsche Untersuchnungen vorgestellt.

  • Invited lecture (Conferences)
    Arbeitstreffen „Kernphysik“ Schleching 2013, 27.2.2013, Schleching, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-18631
Publ.-Id: 18631


Observation of prompt pre-thermal laser ion sheath acceleration and implication on scaling

Zeil, K.; Metzkes, J.; Kluge, T.; Bussmann, M.; Cowan, T.; Kraft, S.; Sauerbrey, R.; Schramm, U.

High-intensity laser-plasma ion generation is promising as a compact, low-cost proton source for applications like ion beam therapy. Using a femtosecond table-top laser system, we studied the intra-pulse phase of the laser driven proton acceleration and show that protons efficiently gain energy in these early times.

  • Lecture (Conference)
    DPG-Frühjahrstagung Dresden, 4.3.2013, Dresden, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-18630
Publ.-Id: 18630


Breit-Wheeler process in very short electromagnetic pulses

Titov, A.; Kämpfer, B.; Takabe, H.; Hosaka, A.

he generalized Breit-Wheeler process, i.e. the emission of $e^+e^-$ pairs off a probe photon propagating through a polarized short-pulsed electromagnetic (e.g.\ laser) wave field, is analyzed. We show that the production probability is determined by the interplay of two dynamical effects. The first one is related to the shape and duration of the pulse and the second one is the non-linear dynamics of the interaction of $e^\pm$ with the strong electromagnetic field. The first effect manifests itself most clearly in the weak-field regime, where the small field intensity is compensated by the rapid variation of the electromagnetic field in a limited space-time region, which intensifies the few-photon events and can enhance the production probability by orders of magnitude compared to an infinitely long pulse. Therefore, short pulses may be considered as a powerful amplifier. The non-linear dynamics in the multi-photon Breit-Wheeler regime plays a decisive role at large field intensities, where effects of the pulse shape and duration are less important. In the transition regime, both effects must be taken into account simultaneously. We provide suitable expressions for the $e^+e^-$ production probability for kinematic regions which can be used in transport codes.

Permalink: https://www.hzdr.de/publications/Publ-18629
Publ.-Id: 18629


Properties of the electron-positron plasma created from vacuum in a strong Laser Field I. Quasiparticle excitations

Blaschke, D.; Kämpfer, B.; Schmidt, S. M.; Panferov, A. D.; Prozorkevich, A. V.; Smolyansky, S. A.

Solutions of a kinetic equation are investigated which describe, on a nonperturbative basis, the vacuum creation of quasiparticle electron-positron pairs due to a strong laser field. The dependence of the quasiparticle electron (positron) distribution function and the particle number density is explored in a wide range of the laser radiation parameters, i.e., the wavelength \lambda and amplitude of electric field strength E_0. Three domains are found: the domain of vacuum polarization effects where the density of the e-e+ pairs is small (the "calm valley"), and two accumulation domains in which the production rate of the e-e+ pairs is strongly increased and the e-e+ pair density can reach a significant value (the short wave length domain and the strong field one). In particular, the obtained results point to a complicated short-distance electromagnetic structure of the physical vacuum in the domain of short wavelengths \lambda \lessim \lambda_{acc} = \pi/m. For moderately strong fields E_0 \lesssim E_c=m^2/e, the accumulation regime can be realized where a plasma with a high density of e-e+ quasiparticles can be achieved. In this domain of the field strengths and in the whole investigated range of wavelengths, an observation of the dynamical Schwinger effect can be facilitated.

Permalink: https://www.hzdr.de/publications/Publ-18628
Publ.-Id: 18628


Investigation on magnetoacoustic properties of spin-ice materials Dy2Ti2O7 and Ho2Ti2O7

Erfanifam, S.; Zherlitsyn, S.; Wosnitza, J.; Moessner, R.; Zvyagin, A. A.; Mcclarty, P.; Petrenko, O.; Balakrishnan, G.

We have investigated elastic properties of the spin-ice materials Dy2Ti2O7 (DTO) and Ho2Ti2O7 (HTO) for a wide range of temperature and magnetic field. Our studies of the sound characteristics for several acoustic modes evidence a renormalization of the sound velocity and the sound attenuation due to phase transformations at applied magnetic field as well as an interaction with low-energy magnetic excitations (topological defects). The most prominent anomalies are quasi-periodic peaks in the sound velocity and in the sound attenuation observed in DTO due to non-equilibrium processes arising in the external magnetic field. These results were analyzed theoretically using exchange-striction coupling, which shows a good agreement between theory and experiment. The obtained results at high magnetic fields exhibit some pronounced anomalies around 50 T for both compounds. Our calculations including crystal-electric field effects show satisfactory agreement with experiment.

  • Lecture (Conference)
    Frühjahrstagung der DPG, 10.-15.03.2013, Regensburg, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-18627
Publ.-Id: 18627


Similarities between the phase diagrams of the S=3/2 Heisenberg spin chains CrXO4 [X=V,P]

Law, J.; Foerster, T.; Glaum, R.; Kremer, R.

CrVO4 and CrPO4 both adopt the same structure type. They can be well described as S=3/2 Heisenberg spin chains with predominant nearest-neighbour only spin exchange interaction. We show here an in-depth investigation into the magnetic structures of both compounds which is complimented by magnetic property measurements. Wherein, we’ve shown that both compounds exhibit a high field phase transition into an unknown state.

  • Lecture (Conference)
    Frühjahrstagung der DPG, 10.-15.03.2013, Regensburg, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-18626
Publ.-Id: 18626


Padé approximations for the magnetic susceptibilities of Heisenberg antiferromagnetic spin chains for various spin values

Law, J.; Kremer, R.

The temperature dependence of the spin susceptibilities of S=1, 3/2, 2, 5/2 and 7/2 Heisenberg nearest-neighbor antiferromagnetic 1D spin chains was simulated via Quantum Monte Carlo calculations, within the temperature range of 0.005 ≤ T⋆ ≤ 100 and fitted to Padé approximations with deviations between the simulated and fitted data of the same order of magnitude or smaller than the Quantum Monte Carlo error. To demonstrate the practicality of our theoretical findings, we successfully compared them with the well known 1D chain compound TMMC (d5, S=5/2) and the new S=1 Heisenberg spin chain NiTa2O6.

  • Lecture (Conference)
    Frühjahrstagung der DPG, 10.-15.03.2013, Regensburg, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-18625
Publ.-Id: 18625


High-Field Magnetotransport in the Electron-Doped Cuprate Superconductor Nd2−xCexCuO4

Helm, T.; Kartsovnik, M. V.; Kampert, E.; Putzke, C.; Biberacher, W.; Grigoriev, P. D.; Baddoux, S.; Proust, C.; Sheikin, I.; Kiswandhi, A.; Brooks, J. S.; Choi, E. S.; Wosnitza, J.; Erb, A.; Gross, R.

es hat kein Abstract vorgelegen

  • Poster
    Frühjahrstagung der DPG, 10.-15.03.2013, Regensburg, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-18624
Publ.-Id: 18624


Investigation of the magnetocaloric effect in La(Fe,Si,Co)13 compound in pulsed magnetic fields

Ghorbani Zavareh, M.; Scurschii, I.; Skokov, K.; Gutfleisch, O.; Wosnitza, J.

es hat kein Abstract vorgelegen

  • Poster
    Frühjahrstagung der DPG, 10.-15.03.2013, Regensburg, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-18623
Publ.-Id: 18623


Spin dynamics in Azurite: high-field ESR studies

Ozerov, M.; Kamenskyi, D.; Wosnitza, J.; Engelkamp, H.; Wolff-Fabris, F.; Francoual, S.; Jaime, M.; Zvyagin, S.

es hat kein Abstract vorgelegen

  • Poster
    Frühjahrstagung der DPG, 10.-15.03.2013, Regensburg, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-18622
Publ.-Id: 18622


AMS measurements of cosmogenic and supernova–ejected radionuclides in deep–sea sediment cores

Feige, J.; Wallner, A.; Fifield, L. K.; Golser, R.; Korschinek, G.; Merchel, S.; Rugel, G.; Winkler, S. R.

Accelerator Mass Spectrometry (AMS) provides the highest sensitivity for measurements of long-lived radionuclides with half-lives in the order of million years. We apply this method to search for live supernova (SN)-produced radionuclides on Earth.

The first indication of a SN close-by to the solar system was published by Knie et al. in 2004. AMS measurements of a ferromanganese crust from the Pacific Ocean showed an excess of 60Fe corresponding to a time some 2 Myr ago. We have obtained two deep-sea sediment cores from the Indian Ocean, which provide a better time resolution due to higher accumulation rates. We use AMS for measuring concentrations of the long-lived radionuclides 26Al, 53Mn and 60Fe in these sediment cores with high time resolution. All three radionuclides, with half-lives between 0.7 and 3.7 Myr, are produced in the late burning phases and during a supernova explosion of a massive star and are ejected into the interstellar medium in the explosion. In contrast to 60Fe, which is not produced in-situ on Earth, cosmogenic production of 26Al and 53Mn in the atmosphere and in-situ adds to a potential extraterrestrial signal. Therefore, accurate data are required for these radionuclides. The cosmogenic isotope 10Be, produced from cosmic rays in the Earth’s atmosphere, is analysed for dating purposes.

We will present our first AMS measurement results for 10Be (DREAMS facility, Germany) and 26Al (VERA, Austria) and will show that, in addition to 10Be, 26Al might be a valuable isotope for dating of deep-sea sediment cores for the past few million years.

Keywords: SN; supernova; AMS; radionuclides

Related publications

  • Lecture (Conference)
    Heavy Ion Accelerator Symposia on Fundamental and Applied Science (HIAS), 08.-12.04.2013, Canberra, Australia

Permalink: https://www.hzdr.de/publications/Publ-18621
Publ.-Id: 18621


Eu valence and Fermi-surface development in EuX2Si2 (X = Co, Rh, Ir) systems

Götze, K.; Seiro, S.; Geibel, C.; Rosner, H.; Petzold, V.; Polyakov, A.; Wosnitza, J.; Sheikin, I.; Suslov, A.

The valence-fluctuating Eu systems EuX2Si2, with X being the transition metal Co, Ir, or Rh, show different types of ground states, strongly depending on X. The instability of the Eu 4f shell underlies this phenomenon and leads among other effects to different valence states ranging from Eu2+ over mixed valence and intermediate valence behavior to Eu3+ [1]. Investigations on the structure and the magnetic behavior of EuCo2Si2, EuIr2Si2, and EuRh2Si2 have revealed their Eu valence. Further experiments on specific heat and resistivity gave insights to magnetic ordering, electronic correlations, and possible valence fluctuations. We report about a systematic de Haas-van Alphen study on the Fermi-surface development of the EuX2Si2 compounds in magnetic fields up to 35 T. High-quality single crystals were available for the first time. We will focus on the Fermi-surface topology obtained by angle dependent measurements and discuss a comparison to band-structure calculations .

  • Lecture (Conference)
    Frühjahrstagung der DPG, 10.-15.03.2013, Regensburg, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-18620
Publ.-Id: 18620


de Haas-van Alphen investigations on the filled skutterudite LaRu4As12 superconductor

Klotz, J.; Götze, K.; Cichorek, T.; Henkie, Z.; Wosnitza, J.

es hat kein Abstract vorgelegen

  • Poster
    Frühjahrstagung der DPG, 10.-15.03.2013, Regensburg, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-18619
Publ.-Id: 18619


Terahertz spectroscopy of superconducting Fe(Se,Te)

Chanda, G.; Pronin, A. V.; Wosnitza, J.; Molatta, S.; Hühne, R.; Holzapfel, B.; Iida, K.

es hat kein Abstract vorgelegen

  • Lecture (Conference)
    Frühjahrstagung der DPG, 10.-15.03.2013, Regensburg, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-18618
Publ.-Id: 18618


Low-Spin Hexacoordinate Mn(III): Synthesis and Spectroscopic Investigation of Homoleptic Tris(pyrazolyl)borate and Tris(carbene)borate Complexes

Forshaw, A.; Smith, J.; Ozarowski, A.; Krzystek, J.; Smirnov, D.; Zvyagin, S.; Harris, T.; Karunadasa, H.; Zadrozny, J.; Schnegg, A.; Holldack, K.; Jackson, T.; Alamiri, A.; Barnes, D.; Telser, J.

Three complexes of Mn(III) with "scorpionate" type ligands have been investigated by a variety of physical techniques. The complexes are Tp2Mn]SbF6 (1), [Tp2*Mn]-SbF6 (2), and [{PhB(MeIm)3}2Mn3 - = phenyltris(3-methylimidazol-2-yl)borate anion. The crystal structure of 3a is reported; the structures of 1 and 2 have been previously reported, but were reconfirmed in this work. The synthesis and characterization of [{PhB(MeIm)3}2Mn]Cl (3b) are also described. These complexes are of interest in that, in contrast to many hexacoordinate (pseudo-octahedral) complexes of Mn(III), they exhibit a low-spin (triplet) ground state, rather than the high-spin (quintet) ground state. Solid-state electronic absorption spectroscopy, SQUID magnetometry, and high-frequency and -field electron paramagnetic resonance (HFEPR) spectroscopy were applied. HFEPR, in particular, was useful in characterizing the S = 1 spin Hamiltonian parameters for complex 1, D = +19.97(1), E = 0.42(2) cm-1, and for 2, D = +15.89(2), E = 0.04(1) cm-1. In addition, frequency domain Fourier-transform THz-EPR spectroscopy, using coherent synchrotron radiation, was applied to 1 only and gave results in good agreement with HFEPR. Variable-temperature dc magnetic susceptibility measurements of 1 and 2 were also in good agreement with the HFEPR results. This magnitude of zero-field splitting (zfs) is over 4 times larger than that in comparable hexacoordinate Mn(III) systems with S = 2 ground states. Complexes 3a and 3b (i.e., regardless of counteranion) have a yet much larger magnitude zfs, which may be the result of unquenched orbital angular momentum so that the spin Hamiltonian model is not appropriate. The triplet ground state is rationalized in each complex by ligand-field theory (LFT) and by quantum chemistry theory, both density functional theory and unrestricted Hartree-Fock methods. This analysis also shows that spin-crossover behavior is not thermally accessible for these complexes as solids. The donor properties of the three different scorpionate ligands were further characterized using the LFT model that suggests that the tris(carbene)borate is a strong sigma-donor with little or no pi-bonding.

Permalink: https://www.hzdr.de/publications/Publ-18617
Publ.-Id: 18617


Magnetic poly(epsilon-caprolactone)/iron-doped hydroxyapatite nanocomposite substrates for advanced bone tissue engineering

Gloria, A.; Russo, T.; D'Amora, U.; Zeppetelli, S.; D'Alessandro, T.; Sandri, M.; Banobre-Lopez, M.; Pineiro-Redondo, Y.; Uhlarz, M.; Tampieri, A.; Rivas, J.; Herrmannsdoerfer, T.; Dediu, V. A.; Ambrosio, L.; de Santis, R.

In biomedicine, magnetic nanoparticles provide some attractive possibilities because they possess peculiar physical properties that permit their use in a wide range of applications. The concept of magnetic guidance basically spans from drug delivery and hyperthermia treatment of tumours, to tissue engineering, such as magneto-mechanical stimulation/activation of cell constructs and mechanosensitive ion channels, magnetic cell-seeding procedures, and controlled cell proliferation and differentiation. Accordingly, the aim of this study was to develop fully biodegradable and magnetic nanocomposite substrates for bone tissue engineering by embedding iron-doped hydroxyapatite (FeHA) nanoparticles in a poly(epsilon-caprolactone) (PCL) matrix. X-ray diffraction analyses enabled the demonstration that the phase composition and crystallinity of the magnetic FeHA were not affected by the process used to develop the nanocomposite substrates. The mechanical characterization performed through small punch tests has evidenced that inclusion of 10 per cent by weight of FeHA would represent an effective reinforcement. The inclusion of nanoparticles also improves the hydrophilicity of the substrates as evidenced by the lower values of water contact angle in comparison with those of neat PCL. The results from magnetic measurements confirmed the superparamagnetic character of the nanocomposite substrates, indicated by a very low coercive field, a saturation magnetization strictly proportional to the FeHA content and a strong history dependence in temperature sweeps. Regarding the biological performances, confocal laser scanning microscopy and AlamarBlue assay have provided qualitative and quantitative information on human mesenchymal stem cell adhesion and viability/proliferation, respectively, whereas the obtained ALP/DNA values have shown the ability of the nanocomposite substrates to support osteogenic differentiation.

Permalink: https://www.hzdr.de/publications/Publ-18616
Publ.-Id: 18616


Superconductivity in Ge and Si via Ga-ion implantation

Skrotzki, R.; Herrmannsdörfer, T.; Schönemann, R.; Heera, V.; Fiedler, J.; Kampert, E.; Wolff-Fabris, F.; Philipp, P.; Bischoff, L.; Voelskow, M.; Mücklich, A.; Schmidt, B.; Skorupa, W.; Helm, M.; Wosnitza, J.

es hat kein Abstract vorgelegen

  • Poster
    Frühjahrstagung der DPG, 10.-15.03.2013, Regensburg, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-18615
Publ.-Id: 18615


Accuracy of 9Be-data and its influence on 10Be cosmogenic nuclide data

Merchel, S.; Bremser, W.; Bourlès, D. L.; Czeslik, U.; Erzinger, J.; Kummer, N.-A.; Leanni, L.; Merkel, B.; Recknagel, S.; Schaefer, U.

A 9Be-solution has been chemically prepared from phenakite (Be2SiO4) mineral grains as commercial 9Be-solutions are too high in long-lived 10Be. The solution is intended to be used as a carrier for radiochemical separation of 10Be to be measured by accelerator mass spectrometry (AMS). Thus, accurate data of the 9Be-concentration of this solution is essential to guarantee for high-accuracy 10Be data in the future. After devastating preliminary results (~8% standard deviation), eight laboratories finally produced twelve individual results by four different analytical methods. A certain lab and method bias might be identified by sophisticated statistical evaluation. Some laboratories also (grossly) underestimate their uncertainties. Thus, the simple weighted mean of this round-robin exercise needed to be corrected by introducing additional allowances (Paule-Mandel-approach). The final result has been calculated to (2246 ± 11) µg 9Be/(g solution) with a reasonably low weighted standard deviation of 0.49%. The maximum deviation of a single lab value from the weighted mean is 2.4% when removing one Grubbs outlier (11% off from the mean) from the data set. As 10Be-data, which is usually calculated from measured 10Be/9Be by AMS and stable 9Be, cannot be more accurate than the determined 9Be-concentration, it seems highly advisable to establish or improve quality assurance by having self-made carrier-solutions analysed at more than a single lab and regularly taking part in round-robin exercises.

Keywords: cosmogenic nuclide; ICP-MS; ICP-OES; AAS; round-robin; accelerator mass spectrometry; AMS

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Permalink: https://www.hzdr.de/publications/Publ-18614
Publ.-Id: 18614


Structure, Optical and Mechanical Properties of Direct Current Magnetron Sputtered Carbon: Vanadium Nanocomposite Thin Films

Krause, M.; Mücklich, A.; Wilde, C.; Vinnichenko, M.; Gemming, S.; Abrasonis, G.

The structure, the optical and the mechanical properties of carbon: vanadium nanocomposite thin films (∼1 at.% to 48 at.% V) grown by direct current magnetron sputtering at 110 °C are investigated using X-ray diffraction, Raman spectroscopy, transmission electron microscopy, spectroscopic ellipsometry, and nano-indentation. At all compositions a phase separation into cubic vanadium carbide, VCx, (x ≤ 1) and carbon is observed, the structure of both phases changing continuously with the vanadium content. The film microstructure consists of statistically distributed spherical VCx particles in a carbon matrix at V concentrations of up to about 35 at.%, and at higher V concentrations of elongated, dendrite-like VCx nanocrystallites, which are separated by a carbon tissue phase. The microstructure hints to a transition from purely repeated nucleation dominated growth to a regime with competing repeated nucleation and surface diffusion. The optical properties are controlled by the phase composition of the films. The hardness is nearly independent of the composition, thus enabling the independent tuning of the absorption behavior at constant hardness.

Related publications

Permalink: https://www.hzdr.de/publications/Publ-18613
Publ.-Id: 18613


Uranium speciation studies at alkaline pH and in the presence of hydrogen peroxide using time-resolved laser-induced fluorescence spectroscopy

Martínez-Torrents, A.; Meca, S.; Baumann, N.; Martí, V.; Giménez, J.; de Pablo, J.; Casas, I.

Time-resolved laser-induced fluorescence spectroscopy (TRLFS) was used to study the speciation of uranium(VI) at very alkaline pH (11–13), at room temperature and in the absence of CO2. In this case, at pH = 11, two different fluorescence lifetimes appeared, which were attributed to the species UO2(OH)3 and (UO2)3(OH)7 . At pH = 13, no fluorescence was detected, indicating that the predominant species, UO2(OH)4 2−, is not fluorescent. At pH = 12, the lifetime obtained is attributed to the predominant species UO2(OH)3 .

Because of the absence of fluorescence of the UO2(OH)4 2− species at room temperature, measurements at 10 K were made, obtaining two different lifetimes in the pH range between 12 and 13.5, indicating the presence of two different species: UO2(OH)3 and UO2(OH)4 2−. The difference between the lifetimes allowed the calculation of the contribution of each species to the total fluorescence signal intensity.

From the experiments carried out in the presence of hydrogen peroxide, it was observed that hydrogen peroxide produces a quenching effect to the fluorescence of the uranium species. At pH 12 the quenching is static, which points to the formation of a non-fluorescent complex between U(VI) and hydrogen peroxide. Using the Stern–Volmer equation for static quenching, the equilibrium formation constant of the first species, UO2O2(OH)2 2−, was calculated to be logK0 = 28.7 ± 0.4, which is similar to the one determined using UV–Visible spectrometry, 28.1 ± 0.2 Meca et al. (2011).

Keywords: Uranium(VI); Speciation; Alkaline pH; Hydrogen peroxide; Cryo-TRLFS; Complex formation constant

Permalink: https://www.hzdr.de/publications/Publ-18612
Publ.-Id: 18612


Investigation of the Magnetic Properties in the Pyrochlore Pr2Sn2O7

Green, E. L.; Herrmannsdörfer, T.; Schönemann, R.; Wang, Z.; Uhlarz, M.; Wosnitza, J.; Zhou, H. D.

  • Lecture (Conference)
    APS March Meeting, 18.-22.03.2013, Baltimore, USA

Permalink: https://www.hzdr.de/publications/Publ-18611
Publ.-Id: 18611


Thermally Excited Ferromagnetic Resonance in MgO-based Magnetic Tunnel Junctions

Kowalska, E.; Bernert, K.; Aleksandrov, Y.; Fowley, C.; Sluka, V.; Mangin, S.; Lindner, J.; Fassbender, J.; Deac, A. M.

Spin polarized currents can exert a so-called spin-transfer torque to the magnetic moment of a ferromagnetic layer. One application of this phenomenon is the spin torque nano-oscillator (typically an MgO-based magnetic tunnel junction (MTJ)) which can act as a tunable microwave emission source. However, a more detailed understanding of the spin-torque physics is needed. For example, the spin torque bias dependence of the two spin torque components (in-plane and fieldlike) is still widely discussed in the community [1]. We present results for MgO-MTJs obtained by thermally excited ferromagnetic resonance (TE-FMR). With the help of TE-FMR, the bias dependence of the two spin-transfer torques can be determined from the peak position and linewidth [2]. Microwave measurements were carried out in the frequency range of 1-9 GHz at positive and negative magnetic fields and for different dc current values. Analyzing this data, we could separate the in-plane and field-like spin torque components and determine their bias dependence.

[1] M. H. Jung et al., PRB 81, 134419 (2010).
[2] A. Deac et al., Nature Phys. 4, 803 (2008).

Keywords: Spin-Transfer Torque; Magnetic Tunnel Junction; Thermally Excited Ferromagnetic Resonance

  • Lecture (Conference)
    DPG Frühjahrstagung 2013, 10.-15.03.2013, Regensburg, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-18610
Publ.-Id: 18610


Towards a statistical treatment of images acquired by automated mineralogy

Birtel, S.; Tolosana Delgado, R.; Matos Camacho, S.; Gutzmer, J.; van den Boogaart, K. G.

A Mineral Liberation Analyzer (MLA) is a scanning electron microscope, delivering quantitative data on mineralogy and microfabric as well as high resolution spatially resolved mineralogical composition images of rock specimen and particle perpetrates (usually grain mounts). MLA images can be processed to extract 2D information, both compositional (modal mineral composition) and microstructural (mineral associations within a particle, average particle diameter distribution, average grain diameter distribution, etc.). Unfortunately, the available software does not fully take into account the limitations of the actual information available: data are collected over a surface while information would actually be required over a volume; and most of them are actually relative, i.e. compositional. Moreover, there is virtually no statistical method or software devised to process data sets of this kind. This contribution presents this kind of data, their particularities and problems, and provides avenues of discussion towards a solution to these issues.

Keywords: mass balances; MLA; stereological reconstruction; stochastic inversion

  • Contribution to proceedings
    15th Annual Conference of International Association of Mathematical Geosciences, 02.-05.09.2013, Madrid, Spain
    Mathematics of Planet Earth, Proceedings of the 15th Annual Conference of IAMG, Heidelberg New York Dorrecht London: Springer, 978-3-642-32407-9, 45-48
    DOI: 10.1007/978-3-642-32408-6
  • Lecture (Conference)
    15th Annual Conference of International Association of Mathematical Geosciences, 02.-05.09.2013, Madrid, Spain

Permalink: https://www.hzdr.de/publications/Publ-18609
Publ.-Id: 18609


Effect of different microorganisms on rare earth phosphors

Kutschke, S.; Hoeppner, N.; Raff, J.; Pollmann, K.

The usage of compact fluorescent lamps (CFLs) increased in the last years. The gas discharge lamps occupy 22% of the German lighting market in 2006 and 41% in 2010. According to the directive 2002/96/EG end-of-life lighting products shall be recycled.
CLFs consist of glass tube, electronic components, rare earth phosphor, and low quantities of mercury. Used discharge lamps should be collected and recycled via specific companies for waste management. Currently, separation of phosphor components is carried out using flotation or acidic leaching. In the present study, alternative leaching of rare earth phosphor using microorganisms was tested. Interaction of algae, pseudomonads, and bacilli with phosphor has been investigated. Results of full factorial plan show, that certain metals are released at specific conditions. Variables of full factorial plan were pH, amount of phosphor and biomass, and time. Chlorella vulgaris, Pseudomonas fluorescens, and Lysinibacillus sphaericus were incubated with the phosphors in shake flasks. The content of released rare earths was analysed in liquid and biomass via ICP-MS. It was observed that main interactions occur with Y and Eu, the rare earth components of red band phosphor.

Keywords: fluorescent phosphor; rare earth; bioleaching; biosorption

  • Contribution to proceedings
    IBS2013 - 20th Internatonal Biohydrometallurgy Symposium, 08.-11.10.2013, Antofagasta, Chile
    Proceedings of the 20th International Biohydrometallurgy Symposium 'Integration of Scientific and Industrial Knowledge on Biohydrometallurgy'

Permalink: https://www.hzdr.de/publications/Publ-18608
Publ.-Id: 18608


Surface speciation of dissolved radionuclides on mineral phases – A vibrational and X-ray absorption spectroscopic study

Foerstendorf, H.; Gückel, K.; Jordan, N.; Rossberg, A.; Brendler, V.

Binary and ternary surface complexes of U(VI) and Np(V) on gibbsite were spectroscopically identified. Se(VI) forms two different types of outer-sphere complexes depending on the solid metal oxide.

Keywords: ATR FT-IR spectroscopy; surface complexes; minerals

Related publications

  • Invited lecture (Conferences)
    5th Asia-Pacific Symposium on Radiochemistry (APSORC 13), 22.-27.09.2013, Kanazawa, Japan

Permalink: https://www.hzdr.de/publications/Publ-18607
Publ.-Id: 18607


High-field magnetization and magnetoelasticity of single crystalline HoFe5Al7

Yasin, S.; Andreev, A. V.; Gorbunov, D.; Skourski, Y.; Zherlitsyn, S.; Wosnitza, J.

es hat kein Abstract vorgelegen

  • Poster
    DPG Frühjahrstagung 2013, 10.-15.03.2013, Regensburg, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-18606
Publ.-Id: 18606


Latest results in the Eu(III)-B(OH)3-Organic System

Schott, J.; Acker, M.; Barkleit, A.; Taut, S.; Brendler, V.; Bernhard, G.

The latest results in the Eu-B(OH)3-Organic System are presented:

1) New approach to determine the formation constant of a Eu borates
2) Formation of the solid Eu borate in NaCl medium
3) Quantitative synthesis of Eu borate and structure characterization

Keywords: Europium; boric acid; borate; polyborate

  • Lecture (Conference)
    Actinidenverbundprojekttreffen, 11.-12.04.2013, Karlsruhe, Germany

Permalink: https://www.hzdr.de/publications/Publ-18605
Publ.-Id: 18605


Entwicklung einer Terminal-Ionenquelle für den 5MV Pelletron-Beschleuniger im Dresdner Felsenkeller

Reinicke, S.; Akhmadaliev, C.; Bemmerer, D.; Zuber, K.

Um astrophysikalisch relevante Wirkungsquerschnitte genau und ohne theoretische Unsicherheiten zu messen, sind Beschleunigerexperimente in geschützten Untertagelabors mit ihrer niedrigen Nullrate oftmals der einzige Weg. Bei Edelgasionen kann zur Erzeugung eines intensiven, hochenergetischen Ionenstrahls aufgrund der geringen Elektronenaffinität kein Tandem-Beschleuniger verwendet werden. Stattdessen werden positive Ionen direkt auf dem Hochspannungsterminal und beim Übergang auf Erdpotential beschleunigt. Der für die Installation im Untertagelabor Felsenkeller vorgesehene 5MV Pelletron-Tandem wird mit einer zusätzlichen Radiofrequenz-Ionenquelle auf dem Terminal ausgerüstet, um intensive Bestrahlungen mit Edelgasionen zu ermöglichen. Der aktuelle Stand zur Konstruktion und zum Einbau der Ionenquelle wird vorgestellt. – Unterstützt von NAVI.

Keywords: Nuclear Astrophysics; Underground experiments; Felsenkeller; ion source; terminal

Related publications

  • Lecture (Conference)
    DPG Frühjahrstagung, 04.-08.03.2013, Dresden, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-18604
Publ.-Id: 18604


Simulation of the Tayler instability in liquid metals

Weber, N.; Galindo, V.; Seilmayer, M.; Stefani, F.; Weier, T.

The Tayler instability, a current driven instability, originally known from plasma physics may appear in liquid metal batteries. We present a numerical model, implemented in OpenFOAM, able to simulate the Tayler instability in incompressible fluids. The finite volume method code, based on the PISO algorithm and enhanced by a Poisson equation for the electric potential and Biot-Savart integration to obtain the induced magnetic field is used to simulate a recent Tayler experiment. Results of field structure and growth rates of the Tayler instability fit well to the experimental findings.

Keywords: FVM OpenFOAM Tayler instability liquid metal battery

  • Lecture (Conference)
    Bifurcations and instabilities in fluid dynamics, 08.-11.07.2013, Haifa, Israel

Permalink: https://www.hzdr.de/publications/Publ-18603
Publ.-Id: 18603


The specific value of junior mining companies: Are common valuation methods appropriate?

Klossek, P.; Klossek, A.

Taking into account the recent worldwide strive for raw materials, the emergence of start-ups in the mining sector for rare metals, and tendencies of financial and strategic investors to invest in such companies, the paper critically evaluates the suitability of common methods widely used to value mining companies. Building on the deficiencies of single methods to capture the specificities of rare earth junior mining companies, which are generally single-project companies, the paper suggests using a combined approach including discounted cash flow, real options, and multipliers methods. Compared to the value obtained by using singular methods, the resulting specific value is argued to better reflect the value of a specific early stage mining company within the rare earth junior mining industry.

Keywords: Junior Mining Company; Start-up; Valuation Method; Rare Earths

Permalink: https://www.hzdr.de/publications/Publ-18602
Publ.-Id: 18602


Application of statistical uncertainty and sensitivity evaluations to a PWR LBLOCA analysis calculated with the code ATHLET. Part 1: Uncertainty analysis

Kozmenkov, Y.; Rohde, U.

Usually, reactor safety analyses are based on the traditional conservative deterministic approach. An alternative approach to reactor safety analyses uses best estimate computer codes in combination with quantification of uncertainties in model and plant parameters. The German Gesellschaft für Anlagen- und Reaktorsicherheit (GRS) has applied the methodology of uncertainty analysis based on the Wilks’ approach. According to this approach, the number of calculations required to perform a probabilistic estimation of an output parameter with a given coverage/confidence level (e.g., 95%/95%) does not depend on the number of input uncertainty parameters. In this paper, the results of an uncertainty analysis for a Large Break LOCA scenario for a generic German PWR of the Konvoi design are reported. All calculations were performed using the system code ATHLET Mod 2.2 Cycle A. The EXCEL-integrated software SUSA developed by GRS was used for generation of the uncertainty parameter vectors, their incorporation into ATHLET input files and for statistical evaluation of the results.

Keywords: Reactor safety analysis; LBLOCA scenario; statistical method; Wilks' theory; ATHLET code; SUSA utility; maximum cladding temperature; upper tolerance limit

  • Kerntechnik 78(2013)4, 354-361

Permalink: https://www.hzdr.de/publications/Publ-18601
Publ.-Id: 18601


Interaction of Eu(III) with Mammalian Cells as a Function of Eu(III) Concentration and Nutrient Composition

Sachs, S.; Heller, A.; Bernhard, G.

In case of the release of long-lived radionuclides, e.g., actinides, into the environment, knowledge about their behavior in biosystems is necessary to assess and prevent health risks for humans. This includes knowledge about bioavailability and toxicity of actinides for/onto cells, which are governed to a large extent by their speciation [1]. In order to enable a better understanding of these processes, we study interaction processes of trivalent actinides/lanthanides with mammalian cells on a cellular level combining biochemical and spectroscopic methods. In the present work we studied the cellular tolerance of FaDu cells (human squamous cell carcinoma cell line) toward Eu(III), as an analog for trivalent actinides, and its uptake into the cells as a function of the metal concentration and the nutrient composition. In parallel, the Eu(III) speciation in the culture media was studied by time-resolved laser-induced fluorescence spectroscopy (TRLFS) to correlate Eu(III) toxicity and uptake with its chemical speciation.

[1] Ansoborlo, E. et al., Biochimie 88 (2006), 1605.

Keywords: Eu(III); europium; interaction; mammalian cells; toxicity; speciation

  • Contribution to proceedings
    The 5th Asia-Pacific Symposium on Radiochemistry '13, APSORC13, 22.-27.09.2013, Kanazawa, Japan
  • Lecture (Conference)
    The 5th Asia-Pacific Symposium on Radiochemistry '13, APSORC13, 22.-27.09.2013, Kanazawa, Japan

Permalink: https://www.hzdr.de/publications/Publ-18600
Publ.-Id: 18600


Large Zero-Field Cooled Exchange-Bias in Bulk Mn2PtGa

Nayak, A. K.; Nicklas, M.; Chadov, S.; Shekhar, C.; Skourski, Y.; Winterlik, J.; Felser, C.

We report a large exchange-bias effect after zero-field cooling the new tetragonal Heusler compound Mn2PtGa from the paramagnetic state. The first-principles calculation and the magnetic measurements reveal that Mn2PtGa orders ferrimagnetically with some ferromagnetic inclusions. We show that ferrimagnetic ordering is essential to isothermally induce the exchange anisotropy needed for the zerofield cooled exchange bias during the virgin magnetization process. The complex magnetic behavior at low temperatures is characterized by the coexistence of a field-induced irreversible magnetic behavior and a spin-glass-like phase. The field-induced irreversibility originates from an unusual first-order ferrimagnetic to antiferromagnetic transition, whereas the spin-glass-like state forms due to the existence of antisite disorder intrinsic to the material.

Permalink: https://www.hzdr.de/publications/Publ-18599
Publ.-Id: 18599


High-field ESR Studies of the Quantum Spin Dimer System Ba3Cr2O8

Kamenskyi, D.; Wosnitza, J.; Krzystek, J.; Aczel, A. A.; Dabkowska, H. A.; Dabkowski, A. B.; Luke, G. M.; Zvyagin, S. A.

Results of systematic high-frequency electron spin resonance (ESR) studies of Ba3Cr2O8, a weakly coupled S = 1/2 dimer system, in magnetic fields up to 25 T are reported. Two pairs of ESR gapped modes corresponding to transitions from a spin-singlet ground state to the first excited triplet states with gaps, ΔAB = 563 GHz and ΔCD = 399 GHz, are revealed below Hc1 = 12.5 T. The detection of the ground-state excitations by means of ESR clearly indicates the presence of a non-secular term allowing these transitions. A complex structure of the microwave absorption spectrum in magnetic fields above Hc1 is observed, those peculiarities are discussed.

Permalink: https://www.hzdr.de/publications/Publ-18598
Publ.-Id: 18598


Emerging evidence for FFLO states in layered organic superconductors

Beyer, R.; Wosnitza, J.

In this short review, we report on the recently found growing experimental evidence for the existence of Fulde–Ferrell–Larkin–Ovchinnikov (FFLO) states in quasi-two-dimensional organic superconductors. At high magnetic fields aligned parallel to the conducting organic layers, we observe an upturn of the upper critical field beyond the Pauli limit, as evidenced by specific-heat and torque-magnetization measurements. Inside the superconducting state a second thermodynamic transition emerges. These features appear only in a very narrow angular region close to parallel-field orientation.

Permalink: https://www.hzdr.de/publications/Publ-18597
Publ.-Id: 18597


Unconventional Magnetostructural Transition in CoCr2O4 at High Magnetic Fields

Tsurkan, V.; Zherlitsyn, S.; Yasin, S.; Felea, V.; Skourski, Y.; Deisenhofer, J.; Krug Von Nidda, H.-A.; Wosnitza, J.; Loidl, A.

The magnetic-field and temperature dependencies of the ultrasound propagation and magnetization of single-crystalline CoCr2O4 have been studied in static and pulsed magnetic fields up to 14 and 62 T, respectively. Distinct anomalies with significant changes in the sound velocity and attenuation are found in this spinel compound at the onset of long-range incommensurate-spiral-spin order at Ts = 27 K and at the transition from the incommensurate to the commensurate states at Tl = 14 K, evidencing strong spinlattice coupling. While the magnetization evolves gradually with the field, steplike increments in the ultrasound clearly signal a transition into a new magnetostructural state between 6.2 and 16.5 K and at high magnetic fields.We argue that this is a high-symmetry phase with only the longitudinal component of the magnetization being ordered, while the transverse helical component remains disordered. This phase is metastable in an extended H - T phase space.

Permalink: https://www.hzdr.de/publications/Publ-18596
Publ.-Id: 18596


High-Field Transitions in ErFe11Ti and HoFe11Ti Single Crystals

Skourski, Y.; Bartolomé, J.; Kuzmin, M. D.; Skokov, K. P.; Bonilla, M.; Gutfleisch, O.; Wosnitza, J.

The magnetization of ErFe11Ti and HoFe11Ti single crystals was measured in pulsed magnetic fields up to 60 T. A number of field-induced phase transitions were observed. The inter-sublattice molecular fields were found to be 60 T in ErFe11Ti and 73 T in HoFe11Ti.

Permalink: https://www.hzdr.de/publications/Publ-18595
Publ.-Id: 18595


Magnet-Technology Development at the Dresden High Magnetic Field Laboratory

Zherlitsyn, S.; Wustmann, B.; Herrmannsdörfer, T.; Wosnitza, J.

The Dresden High Magnetic Field Laboratory (HLD) is a user facility which provides scientists with the possibility to perform a broad range of experiments in pulsed magnetic fields. Recent progress in the magnet-technology development at the HLD has led to significant advances in achieving non-destructive pulsed magnetic fields close to the megagauss mark. Using 9.5 MJ dual-coil magnets with 16 mm bore, in 2011 a world-record field of 91.4 T has been achieved. Later 94.2 T have been reached.We report on the magnet design and performance of these magnets as well as on the design for the next generation of dual-coil magnets characterized by interchangeable inner sub-coils and improved control of the axial preload.

Permalink: https://www.hzdr.de/publications/Publ-18594
Publ.-Id: 18594


Field-Induced Gap in the Spin-1/2 Heisenberg Chain Compound Cu-Pyrimidine Dinitrate: ESR Studies in Magnetic Fields up to 63 T

Ozerov, M.; Wosnitza, J.; Cižmár, E.; Feyerherm, R.; Manmana, S. R.; Mila, F.; Zvyagin, S. A.

Results of electron spin resonance studies of copper pyrimidine dinitrate (Cu-PM, [PM-Cu(NO3)2(H2O)2]n, PM= pyrimidine), a spin-1/2 antiferromagnetic chain material with alternating g-tensor and Dzyaloshinskii-Moriya interactions, in pulsed magnetic fields up to 63 T are reported. The field-induced gap shows a nonmonotonic behavior with a minimum in the vicinity of the saturation field Hsat = 48.5 T. This is associated with a transition from the sine-Gordon region to a spinpolarized state with magnon excitations. By comparing the entire set of experimental data with results of density matrix renormalization group calculations for Cu-PM, the validity of the used theoretical approach is proven.

Permalink: https://www.hzdr.de/publications/Publ-18593
Publ.-Id: 18593


Investigations of the sorption of U(VI) onto SiO2 in the presence of phosphate: In search of a ternary surface complex

Comarmond, M. J.; Foerstendorf, H.; Steudtner, R.; Chong, E.; Heim, K.; Müller, K.; Gückel, K.; Brendler, V.; Payne, T. E.

The adsorption of U(VI) in the environment is known to be influenced by the presence of both inorganic and organic ligands in the aqueous phase [1]. In the present study, the ternary system containing U(VI), phosphate and SiO2 is investigated using a batch sorption technique, in situ attenuated total reflection Fourier-transform infrared (ATR FT-IR) spectroscopy and time-resolved laser-induced fluorescence spectroscopy (TRLFS). Whilst SiO2 is a predominant component of soils and host rock and the speciation of uranium with phosphate is complex [2], limited studies of the U(VI)/PO4/SiO2 ternary system [3] exist. Nevertheless, such studies have significant relevance in understanding radionuclide migration in geological systems.

[1] Payne, T.E., Lumpkin, G.R. and Waite, T.D. (1998). ‘UraniumVI adsorption on model minerals” in Adsorption of Metals by Geomedia, Chapter 2, p. 75-97, Jenne, E.A., Ed.; Academic Press, San Diego, U.S.A.
[2] Sandino, A. and Bruno, J. (1992). “The solubility of (UO2)3(PO4)2.4H2O(s) and the formation of U(VI) phosphate complexes: Their influence in uranium speciation of natural waters.” Geochimica et Cosmochimica Acta, 56, 4135-4145.
[3] Zhang, H. and Tao, Z. (2002). “Sorption of uranyl ions on silica: Effects of contact time, pH, ionic strength, concentration and phosphate.” Journal of Radioanalytical and Nuclear Chemistry 254(1), 103-107.

Keywords: ATR FT-IR; TRLFS; Uranium; Speciation

  • Poster
    14th International Conference on the Chemistry and Migration Behaviour of Actinides and Fission Products in the Geosphere, 08.-13.09.2013, Brighton, United Kingdom

Permalink: https://www.hzdr.de/publications/Publ-18592
Publ.-Id: 18592


On the impact of potential processing technology developments on rare earth mining economics

Klossek, P.; van den Boogaart, K. G.

It is estimated that China accounts for 94% of the world supply of rare earths (Roskill, 2011). This fact, together with the impact of China’s export policy, poses a substantial risk to the security of the rare earth supply as well as a rare earth price risk. This situation has motivated an increase in the number of rare earth projects under development, i.e., there are currently more than 440 worldwide (Technology Metals Research, 2012). However, economically and environmentally acceptable processing technology to produce tradable products from rare earths (e.g., separated rare earth oxides) is not freely available on the market at the moment. In this respect, a lot of research and development has been initiated on this topic, in academia as well as in industry. Using a proprietary model and scenario-based analysis, we studied the impact that the development of rare earth processing technologies would have on the rare earth market and the economic feasibility of rare earth projects mentioned before. The analysis showed that this impact varies depending on the technology type (e.g., technology can affect project production volume, cost structure or both) and the legal context of the invention (e.g., free or limited by patenting availability of a new technology). The effect of a technology which influences project production volume is not the same as of a technology which changes project cost structure. The impact of a patented processing technology differs from the impact of a processing technology which is freely available on the market. In the case of a new technology which is limited by patenting, its impact depends on the market position (“producing”, “next-coming”, or “not producing” project) of the patent holder. The paper contributes to existing research by studying the dependence of the expected micro- and macroeconomic impact of rare earth processing technology developments on the properties of a new technology (e.g., costs, legal framework etc.). By this means, the paper adds to existing knowledge and attempts to make the rare earths market more transparent and predictable from a perspective outside China.

Keywords: Processing Technology; Mining Economics; Rare Earths

  • Contribution to proceedings
    23rd World Mining Congress, 11.-15.08.2013, Montreal, Canada
    Proceedings of the 23rd World Mining Congress
  • Lecture (Conference)
    23rd World Mining Congress, 11.-15.08.2013, Montreal, Canada

Permalink: https://www.hzdr.de/publications/Publ-18591
Publ.-Id: 18591


Economic evaluation as a critical part of the mine development process: The case of rare earths

Klossek, P.; van den Boogaart, K. G.

Mine development cannot progress without observing positive results of economic evaluation, which is the potential profitability of a future mine. According to the discounted cash flow (DCF) method, i.e., the most widely used method in mining, net present value is generally calculated as an indicator of project profitability. However, in the case of critical metals, e.g., rare earth elements (REE), the required for the economic calculations data is problematic to be generated. This is due to the specific features of these metals which also complicate economic evaluation of corresponding projects. Using the recent example of REE the paper explains how exactly their specific features complicate economic evaluation. We suggest possible solutions which include the extension of the DCF method, e.g., by the additional application of game theory, as well as the use of alternative methods, e.g., real options. Finally, we discuss the need for an integrated approach to economic evaluation of REE projects.

Keywords: Mine development; economic evaluation; rare earths

  • Contribution to proceedings
    4th International Conference Mineral Resources and Mine Development - AIMS 2013, 22.-23.05.2013, Aachen, Germany
    Proceedings of the 4th International Conference Mineral Resources and Mine Development, Essen: Verlag Glückauf GmbH, 978-3-86797-154-6, 249-256
  • Lecture (Conference)
    4th International Conference Mineral Resources and Mine Development - AIMS 2013, 22.-23.05.2013, Aachen, Germany

Permalink: https://www.hzdr.de/publications/Publ-18590
Publ.-Id: 18590


Radiolabeled COX-2 inhibitors for non-invasive visualization of COX-2 expression and activity - a critical update

Laube, M.; Kniess, T.; Pietzsch, J.

Cyclooxygenase-2 (COX-2) is a key player in inflammation. Its overexpression is directly associated with various inflammatory diseases and, additionally, with several processes of carcinogenesis. The development of new selective COX-2 inhibitors (COXIBs) for use in cancer treatment is in the focus of the medicinal chemistry research field. For this purpose, a set of methods is available to determine COX-2 expression and activity in vitro and ex vivo but it is still a problem to functionally characterize COX-2 in vivo. This review focusses on imaging agents targeting COX-2 which have been developed for positron emission tomography (PET) and single photon emission computed tomography (SPECT) since 2005. The literature reveals that different radiochemical methods are available to synthesize COXIBs radiolabeled with fluorine-18, carbon-11, and isotopes of radioiodine. Unfortunately, most of the compounds tested did not show sufficient stability in vivo due to de[18F]fluorination or de[11C]methylation or they failed to bind specifically in the target region. So, suitable stability in vivo, matching lipophilicity for the target compartment and both high affinity and selectivity for COX-2 were identified as prominent criteria for radiotracer development. Up to now, it is not clear what approach and which model is the most suited to evaluate COX-2 targeting imaging agents in vivo. However, for proof of principle it has been shown that some radiolabeled compounds can bind specifically in COX-2 overexpressing tissues which gives hope for future work in this field.

Keywords: cyclooxygenase; inhibitor; imaging; visualization; radionuclide; fluorine-18; carbon-11; radioiodine; COXIB; NSAID

Permalink: https://www.hzdr.de/publications/Publ-18589
Publ.-Id: 18589


3D Analysis of fluid flow in fissured salt rock

Wolf, M.; Enzmann, F.; Kulenkampff, J.; Lippmann-Pipke, J.

The processes of dissolution and destabilization during and right after the flooding of a salt mine are in principle well understood but in detail still enigmatic. In our attempt to visualize these mechanisms, a combination of structural imaging as well as computer simulations were performed at the pore scale. High resolution positron emission tomography in situ imaging of fluid flow processes in heterogeneously structured drilling cores were matched with high resolution x-ray computer tomography imaging of effective hydraulic microstructures [1]. The microstructures were used as input for lattice Boltzmann based particle tracking simulations [2]. The space and time resolved combined imaging of hydraulic effective structures and fluid flow processes (Figure 1) allows an estimation of the effective volume within the network of pores and fissures and an estimation of the reactive surface area of rock material. Flow path topology concerning, e.g., fingering phenomena, dispersion and molecular diffusion effects can be quantified, and velocity distribution can be observed in 3D [3].

With PET, we observed the propagation of brine labelled with a PET-tracer (124I or 18F) through a mechanically damaged rock salt drill core, which was structurally characterized with CT. The experiments show, that two heterogeneous effects have to be considered with respect to dissolution and destabilization of the material. The first one is a strong localization of fluid paths dominated by fingering phenomena especially along fissures but also in parts in homogeneous porous areas. As a consequence, fluid in motion uses only a small part of the available pathway even under saturated conditions. The fraction of the internal surface of a rock sample which is exposed to the propagating fluid – the effective reactive surface area – decreases with increasing localization of actual transport paths. Therefore, this effect considerably narrows the part of the pore space, where dissolution or other interactions are likely to occur. This effective pore volume and surface area can be quantified experimentally with PET process observation and with CT-based flow field simulations. The second mechanism is a high variability in the streaming velocity patterns along distinct parts of the fractures. Locally enhanced flow velocities increase local dissolution and cause widening of fracture cross sections. This may lead to a self-enhancing effect of increasing flow velocities and flow rates in saline rock. These results may contribute to the understanding of destabilization and dissolution processes and ultimately pylon collapse upon flooding of a salt mine.

  • Lecture (Conference)
    Migration conference 2013 - 14th International Conference on the Chemistry and Migration Behaviour of Actinides and Fission Products in the Geosphere, 08.-13.09.2013, Brighton, United Kingdom

Permalink: https://www.hzdr.de/publications/Publ-18588
Publ.-Id: 18588


Photoresponse from single upright-standing ZnO nanorods explored by photoconductive AFM

Beinik, I.; Kratzer, M.; Wachauer, A.; Wang, L.; Piryatinski, Y. P.; Brauer, G.; Chen, X. Y.; Hsu, Y. F.; Djurisic, A.; Teichert, C.

ZnO nanostructures are promising candidates for the development of novel electronic devices due to their unique electrical and optical properties. Here, photoconductive atomic force microscopy (PC-AFM) has been applied to investigate transient photoconductivity and photocurrent spectra of upright-standing ZnO nanorods (NRs). With a view to evaluate the electronic properties of the NRs and to get information on recombination kinetics, we have also performed time-resolved photoluminescence measurements macroscopically.

Keywords: ZnO nanorods; photoconductive atomic force microscopy; transient photoconductivity and photocurrent spectra

Permalink: https://www.hzdr.de/publications/Publ-18587
Publ.-Id: 18587


Investigation of dynamic liquid distribution and hold-up in structured packings using ultrafast electron beam X-ray tomography

Janzen, A.; Schubert, M.; Barthel, F.; Hampel, U.; Kenig, E. Y.

Dynamic cross-sectional liquid distribution and hold-up in a DN80 separation column filled with structured packings was studied using an ultrafast electron-beam X-ray tomograph with high temporal resolution of 2000 images per second. The modality allows visualisation and characterisation of the counter-current flow before and at the flooding point representing the upper operation limit. Two packings of the same type (Montz B1-MN) with different specific surface area were used to investigate the influence of the packing geometry on the spatial liquid distribution. The system studied was water/air at different gas and liquid loads. The results of the tomographic imaging and corresponding post-processing routines were validated by comparison with conventional draining measurements.

Keywords: Structured packing; Separation column; Dynamic liquid distribution; Ultrafast X-ray tomography; Liquid hold-up; Flooding conditions

Permalink: https://www.hzdr.de/publications/Publ-18586
Publ.-Id: 18586


Modeling of transition phenomena for bubbles columns and validating with CFD

Ziegenhein, T.; Krepper, E.; Rzehak, R.; Lucas, D.

Coalescence and break-up are complex (local) effects which depend on turbulence, shear rate, bubble sizes/polydispersity, local void fraction, bubble shape and material properties
- Complete modeling of all effects that influence these parameters is necessary
- Goal: Defining a general baseline model which covers the effects of bubbly flow

Keywords: Bubble column; CFD Simulation; Multiphase flow; Coalescence

  • Poster
    Jahrestreffen der Fachgruppen Extraktion und Mehrphasenströmungen, 19.-20.03.2013, Baden-Baden, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-18585
Publ.-Id: 18585


Closure relations for CFD simulation of bubble columns

Ziegenhein, T.; Lucas, D.; Rzehak, R.; Krepper, E.

This paper describes the modelling of bubbly flow in a bubble column considering non-drag forces, polydispersity and bubble induced turbulence using the Eulerian two-fluid approach. The set of used closure models describing the momentum exchange between the phases was chosen on basis of broad experiences in modelling bubbly flows at the Helmholtz-Zentrum Dresden-Rossendorf. Polydispersity is modeled using the inhomogeneous multiple size group (iMUSIG) model, which was developed by ANSYS/CFX and Helmholtz-Zentrum Dresden-Rossendorf. Through the importance of a comprehensive turbulence modeling for coalescence and break-up models, bubble induced turbulence models are investigated. A baseline has been used which was chosen on the basis of our previous work without any adjustments. Several variants taken from the literature are shown for comparison. Transient CFD simulations are compared with the experimental measurements and Large Eddy Simulations of Akbar et al. (2012).

Keywords: Bubble column; two-fluid model; bubble forces; bubble induced turbulence

  • Contribution to proceedings
    International Conference on Multiphase Flow 2013, 26.-31.05.2013, Jeju, Korea
  • Lecture (Conference)
    International Conference on Multiphase Flow 2013, 26.-31.05.2013, Jeju, Korea

Permalink: https://www.hzdr.de/publications/Publ-18584
Publ.-Id: 18584


Numerical simulation of polydispersed flow in bubble columns with the inhomogeneous Multi-Size-Group (iMUSIG) model

Ziegenhein, T.; Rzehak, R.; Krepper, E.; Lucas, D.

The present paper shows the influence of considering polydispersity of bubbly flow, simulating bubble columns with a three-dimensional Eulerian two-fluid model. A complete set of interfacial closure models regarding drag force, lift force, wall force, turbulent dispersion force and bubble induced turbulence is considered. A round bubble column of 0.288 m diameter and 2.5 m height is simulated up to a superficial gas velocity of 1 cm/s and compared with experimental data. It is shown that considering the polydispersity including the non-drag forces, important flow properties of bubble columns are reproduced. Possible influences of swarm effects on the non-drag forces are discussed and needs for further investigations are given.

Keywords: bubble column hydrodynamics; homogeneous flow regime; dispersed multiphase flow; Eulerian two fluid; CFD simulation; model validation

Permalink: https://www.hzdr.de/publications/Publ-18583
Publ.-Id: 18583


Laser-driven particle accelerators for radiotherapy

Metzkes, J.; Baumann, M.; Beyreuther, E.; Burris-Mog, T.; Bussmann, M.; Cowan, T. E.; Enghardt, W.; Karsch, L.; Kluge, T.; Kraft, S. D.; Kroll, F.; Laschinsky, L.; Masood, U.; Oppelt, M.; Pawelke, J.; Richter, C.; Sauerbrey, R.; Schramm, U.; Schürer, M.; Siebold, M.; Zeil, K.

  • Poster
    Evaluation of the Helmholtz Program Cancer Research 2013, 18.-20.03.2013, Heidelberg, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-18582
Publ.-Id: 18582


Inclusive pion and eta production in p+Nb collisions at 3.5 GeV beam energy

Agakishiev, G.; Balanda, A.; Belver, D.; Belyaev, A.; Berger-Chen, J. C.; Blanco, A.; Böhmer, M.; Boyard, J. L.; Cabanelas, P.; Chernenko, S.; Dybczak, A.; Epple, E.; Fabbietti, L.; Fateev, O.; Finocchiaro, P.; Fonte, P.; Friese, J.; Fr¨Ohlich, I.; Galatyuk, T.; Garz´On, J. A.; Gernhäuser, R.; Göbel, K.; Golubeva, M.; Gonzalez-Diaz, D.; Guber, F.; Gumberidze, M.; Heinz, T.; Hennino, T.; Holzmann, R.; Ierusalimov, A.; Iori, I.; Ivashkin, A.; Jurkovic, M.; Kämpfer, B.; Karavicheva, T.; Koenig, I.; Koenig, W.; Kolb, B. W.; Kornakov, G.; Kotte, R.; Krasa, A.; Krizek, F.; Krücken, R.; Kuc, H.; Kühn, W.; Kugler, A.; Kurepin, A.; Ladygin, V.; Lalik, R.; Lang, S.; Lapidus, K.; Lebedev, A.; Liu, T.; Lopes, L.; Lorenz, M.; Maier, L.; Mangiarotti, A.; Markert, J.; Metag, V.; Michalska, B.; Michel, J.; Müntz, C.; Naumann, L.; Pachmayer, Y. C.; Palka, M.; Parpottas, Y.; Pechenov, V.; Pechenova, O.; Pietraszko, J.; Przygoda, W.; Ramstein, B.; Reshetin, A.; Rustamov, A.; Sadovsky, A.; Salabura, P.; Schmah, A.; Schwab, E.; Siebenson, J.; Sobolev, Y. G.; Spataro, S.; Spruck, B.; Ströbele, H.; Stroth, J.; Sturm, C.; Tarantola, A.; Teilab, K.; Tlusty, P.; Traxler, M.; Trebacz, R.; Tsertos, H.; Vasiliev, T.; Wagner, V.; Weber, M.; Wendisch, C.; Wüstenfeld, J.; Yurevich, S.; Zanevsky, Y.

Data on inclusive pion and eta production measured with the dielectron spectrometer HADES in the reaction p+93Nb at a kinetic beam energy of 3.5 GeV are presented. Our results, obtained with the photon conversion method, supplement the rather sparse information on neutral meson production in proton-nucleus reactions existing for this bombarding energy regime. The reconstructed e+e−e+e− transverse-momentum and rapidity distributions are confronted with transport model calculations which account well for pi0 but deviate for eta.

Permalink: https://www.hzdr.de/publications/Publ-18581
Publ.-Id: 18581


Phase-Resolved X-ray Ferromagnetic Resonance Measurements of Spin Pumping in Spin Valve Structures

Marcham, M. K.; Shelford, L. R.; Cavill, S. A.; Keatley, P. S.; Yu, W.; Shafer, P.; Neudert, A.; Childress, J. R.; Katine, J. A.; Arenholz, E.; Telling, N. D.; van der Laan, G.; Hicken, R. J.

Element-specific phase-resolved x-ray ferromagnetic resonance (FMR) was used to study spin pumping within Co50Fe50(3)/ Cu(6)/ Ni80Fe20(5) (thicknesses in nm) spin valve structures with large areas, so that edge effects typical of nanopillars used in standard magnetotransport experiments could be neglected. The phase of precession of the Co50Fe50 fixed layer was recorded as FMR was induced in the Ni80Fe20 free layer. The field dependence of the fixed layer phase contains a clear signature of spin transfer torque (STT) coupling due to spin pumping. Fitting the phase delay yields the spin mixing conductance, the quantity that controls all spin transfer phenomena. The STT coupling is destroyed by insertion of Ta into the middle of the Cu layer.

Keywords: XMCD; FMR; XFMR

Permalink: https://www.hzdr.de/publications/Publ-18580
Publ.-Id: 18580


Sorption of selenium oxyanions onto hematite

Jordan, N.; Domaschke, S.; Foerstendorf, H.; Scheinost, A. C.; Weiß, S.; Heim, K.

The 79Se isotope, which is a long-lived (t1/2 ~ 3.27 × 105 years[1]) and radiotoxic fission product found in spent nuclear fuels, is of high importance in the context of geological disposal facilities. Safety calculations assessments have shown it to be one of the most contributing isotopes to the total radioactivity that could be potentially released to the biosphere. Selenium has a quite complex speciation, with four main oxidation states, depending on both the pH and the redox potential of the surrounding environment. The concentration, the bioavailability, the mobility, the distribution and the oxidation state of selenium in the environment are greatly influenced by the pH, nature of mineral sorbent as well as potential redox reactions at mineral surfaces. Among the mechanisms which enable selenium retardation and reduces its migration, adsorption processes onto solid surfaces (iron, alumina, titanium oxides) has been extensively investigated at room temperature [2-4].
Our study focuses on selenium(VI) and selenium(IV) sorption onto hematite (α-Fe2O3), which was so far not thoroughly characterized yet. By means of EXAFS and ATR FT-IR spectroscopic studies, it was observed that selenium(VI) forms purely monodentate inner-sphere complexes onto hematite, but the study was only performed at pD 3.5 [5]. To our knowledge, the only spectroscopic characterization of the binary selenium(IV)/hematite system concluded the formation of bidentate bridging inner-sphere complexes onto single hematite crystal using x-ray standing wave (XSW), but the measurements were only performed at pH 4.0 [6]. Hematite was chosen because it is a ubiquitous iron oxide mineral present in the environment. In addition, it is an iron phase often found in rocks and soils in the vicinity of underground repositories [7]).
At the macroscopic level, the effect of pH and ionic strength was studied by means of batch experiments. Sorption of both oxyanions was found to decrease with increasing pH. An increase of the ionic strength (from 0.01 M to 0.1 M) impacted the sorption of selenium(VI), while the selenium(IV) uptake was found to be not significantly affected. Electrophoretic mobility measurements revealed that selenium(IV) sorption shifted the isoelectric point (pHIEP) of hematite to lower pH values, while the pHIEP was not significantly modified upon selenium(VI) sorption. At the molecular level, in situ ATR FT-IR measurements revealed the formation of inner-sphere complexes during selenium(IV) sorption onto hematite, while the sorption of selenium(VI) proceeded via the formation of outer-sphere complexes. Complementary information about the Se reactivity at the hematite surface is provided by EXAFS spectroscopy.
High level and long-lived radioactive wastes are well-known to increase the temperature at the vicinity of the waste disposal site. Such a thermal effect raises the question how the retention of selenium is influenced at elevated temperatures. By means of batch sorption experiments, electrophoretic mobility measurements and in situ ATR FT-IR spectroscopic studies, information and insights about mechanisms involved at higher temperatures (from 25 °C to 60 °C) are provided.

[1] G. Jörg, R. Buhnemann, S. Hollas, N. Kivel, K. Kossert, S. Van Winckel, C.L.V. Gostomski, Appl. Radiat. Isotopes 68 (2010) 2339.
[2] E.J. Elzinga, Y.Z. Tang, J. McDonald, S. DeSisto, R.J. Reeder, J. Colloid Interface Sci. 340 (2009) 153.
[3] N. Jordan, A. Ritter, H. Foerstendorf, A.C. Scheinost, S. Weiss, K. Heim, J. Grenzer, A. Mucklich, H. Reuther, Geochim. Cosmochim. Acta 103 (2013) 63.
[4] A.C. Scheinost, L. Charlet, Environmental Science & Technology 42 (2008) 1984.
[5] D. Peak, D.L. Sparks, Environ. Sci. Technol. 36 (2002) 1460.
[6] J.G. Catalano, Z. Zhang, P. Fenter, M.J. Bedzyk, J. Colloid Interface Sci. 297 (2006) 665.
[7] F. Claret, B.A. Sakharov, V.A. Drits, B. Velde, A. Meunier, L. Griffault, B. Lanson, Clay Clay Min. 52 (2004) 515.

Keywords: selenium; sorption; hematite; ATR FT-IR; EXAFS; temperature

Related publications

  • Contribution to proceedings
    14th International Conference on the Chemistry and Migration Behaviour of Actinides and Fission Products in the Geosphere, 08.-13.09.2013, Brighton, United Kingdom
    Proceedings of the Migration Conference 2013

Permalink: https://www.hzdr.de/publications/Publ-18579
Publ.-Id: 18579


Study of Europium and Nickel interaction with calcite - batch experiments and spectroscopic characterization

Sabău, A.; Jordan, N.; Lomenech, C.; Marmier, N.; Brendler, V.; Barkleit, A.; Surblé, S.; Toulhoat, N.; Pipon, Y.; Moncoffre, N.; Giffaut, E.

Interactions between cations and natural or synthetic calcite may include incorporation processes, resulting in the irreversibility of some sorption reactions. Calcite is present in soil and sediment materials, and in particular in the Callovo-Oxfordian clay samples from of the French underground laboratory of Bure (France), studied in the context of an underground repository for radioactive waste. Europium has been chosen to be investigated by TRLFS due to its fluorescent properties and because it can serve as an analogue for trivalent actinides. Nickel is toxic as a heavy metal as well as in its radioactive form. Few experimental studies have been made to define its interaction with soil and sediment minerals in general and only a handful of articles report investigations of Ni interaction with calcite. To investigate these irreversible processes, we have chosen to work on the Eu-CO2-NaCl-CaCO3 and Ni-CO2-NaCl-CaCO3 systems at pH 8.4, buffered by calcite under atmospheric conditions.
Our study combines macroscopic batch experiments with spectroscopic investigations (Time Resolved Laser Fluorescence Spectroscopy - TRLFS and Rutherford Backscattering Spectrometry - RBS) to comprehensively characterize these systems.

First, appropriate material for sorption experiments were selected based on characterization studies. Eventually, a calcite powder from SOLVAY (SOCAL U1-R) with a particle size of 0.2 μm for TRLFS investigations was chosen, mainly due to its large BET specific surface area (i.e. 18.4 m2/g). In addition, a calcite powder from OMYA (BL 200), with a bigger particle size (56 μm) and a lower specific surface area (0.7 m2/g) was used for Rutherford Backscattering Spectrometry (RBS) measurements, due to the specific requirements of this technique.
For both powders, Diffuse Reflectance Infra-Red Fourier Transform Spectroscopy (DRIFT), X-ray Diffraction (XRD), Scanning Electron Microscopy (SEM) and elementary analysis confirmed the absence of polymorphic CaCO3 compounds (i.e. vaterite and aragonite).
In order to get a better understanding of incorporation of cations in the structure of calcite, we compared our results obtained on powders with studies on millimetric calcite single crystals from Alfa Aesar, performed under the same experimental conditions as for powders.
The sample preparation consists in open reactor experiments under atmospheric conditions (pCO2 = 10-3.5 atm) in 0.1 M NaCl media. The studied concentrations range from 10-6 to 10-3 M. The experiments were carried out for contact times ranging from 4 hours to 6 months for europium and from 4 hours up to 3 months for nickel. For europium, ICP-AES/ICP-MS analysis of the supernatants showed a strong retention by calcite whatever the initial concentration, contrary to nickel where the retention is depending on the initial concentration.

The second step of the work involved efforts to better understand the time-dependence of Eu and Ni sorption and respective mechanisms.
For each concentration of europium investigated by TRLFS, two species are identified and their fluorescence lifetime increases as the initial concentration decreases and time goes on, corresponding to a gradual loss of water molecules surrounding the europium. For higher concentrations, the species identified appear to correspond to a (co-) surface precipitate and possibly an inner-sphere surface complex with two water molecules retained in the hydration sphere. For lower concentrations, the longer lifetimes observed for one of the two species suggest the incorporation of europium in calcite [1,2].
Rutherford Backscattering Spectrometry (RBS) experiments have been carried out using an alpha particle millibeam at the 4MV Van de Graaff accelerator of IPNL and also on nuclear microprobe of CEA-Saclay. This technique is well adapted to discriminate sorption processes such as: (i) adsorption or co precipitation at the mineral surfaces or (ii) incorporation into the mineral structure (through diffusion for instance). The interpretation of the results shows different sorption behaviors for Ni and Eu. Ni accumulates at the calcite surface whereas Eu is also incorporated at a greater depth. Eu seems therefore to be incorporated into two different states in calcite: (i) heterogeneous surface accumulation, which confirms the hypothesis of the surface precipitate, and (ii) incorporation up to depths greater than 160 nm after 1 month of sorption. Complementary Scanning Electron Microscopy (SEM) observations of the mineral surfaces at low voltage have also been carried out, which confirmed the heterogeneities detected by RBS measurements.

[1] Fernandes, M. M.; Schmidt, M.; Stumpf, T.; Walther, C.; Bosbach, D.; Klenze, R.; Fanghänel, Th., Journal of Colloid and Interface Science (2008), 321(2), 323-331.
[2] Piriou, B; Fedoroff, M.; Jeanjean, J.; Bercis, L., Journal of Colloid and Interface Science (1997), 194, 440-447.

Keywords: Europium; Nickel; calcite; incorporation; diffusion; TRLFS; RBS

  • Poster
    14th International Conference on the Chemistry and Migration Behaviour of Actinides and Fission Products in the Geosphere, 08.-13.09.2013, Brighton, United Kingdom

Permalink: https://www.hzdr.de/publications/Publ-18578
Publ.-Id: 18578


On the geological availability of germanium

Frenzel, M.; Ketris, M. P.; Gutzmer, J.

Based on a detailed statistical analysis of chemical data published in the scientific literature, estimates were made of the minimum amounts of recoverable Ge contained within sulphidic zinc ores and coals, given current processing technologies. It is expected that at least 119 kt (∼7 kt in zinc ores and ∼112 kt in coal) of recoverable germanium exist within proven reserves (at present stage of knowledge) at grades in excess of 100 ppm in sphalerite and 200 ppm in coal, while at least 440 kt (∼50 kt in zinc ores and ∼390 kt in coal) should become recoverable in the future, being associated to coal reserves at 8–200 ppm Ge and zinc resources containing in excess of 100 ppm Ge in sphalerite. Mississippi Valley Type (MVT) deposits are expected to be the most important hosts of germanium-rich sphalerite, while both brown and hard coals are expected to be equally important as hosts of germanium. The approach taken in this publication shows that reliable minimum estimates for the availability of by-product metals lacking suitable reserve/resource data may be attained by using robust statistical methods and geochemical data published in the scientific literature.

Keywords: critical metals; resources; reserves; sphalerite; coal

Permalink: https://www.hzdr.de/publications/Publ-18577
Publ.-Id: 18577


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