Publications Repository - Helmholtz-Zentrum Dresden-Rossendorf
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43566 Publications
Photodisintegration of the p-nuclei 92Mo and 144Sm in the astrophysically relevant energy window
Nair, C.; Erhard, M.; Junghans, A. R.; Bemmerer, D.; Beyer, R.; Grosse, E.; Klug, J.; Kosev, K.; Rusev, G.; Schilling, K. D.; Schwengner, R.; Wagner, A.
Abstract
The heavy neutron deficient p-nuclei are produced in explosive stellar environments via photodisintegration reactions like (g ,n), (g ,p) and (g ,alpha) on r- or s- seed nuclei. The reaction rates of p-nuclei are mostly based on theoretical parameterizations using statistical model calculations. We study experimentally the photodisintegration rates of heavy nuclei at the bremsstrahlung facility of the superconducting electron accelerator ELBE of FZ Dresden-Rossendorf. Photoactivation measurements on the astrophysically relevant p-nuclei 92Mo and 144Sm have been performed with bremsstrahlung end-point energies from 10.0 to 16.5 MeV. The activation yields are compared with calculations using cross sections from recent Hauser-Feshbach models. The sensitivity of the statistical models to the input ingredients like photon strength function, optical potentials are tested against the experimental activation yield.
Keywords: photodisintegration; p-nuclei; photoactivation
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Contribution to proceedings
International conference Nuclei in Cosmos- X, 27.07.-01.08.2008, Mackinac Island, Michigan, United States
Photodisintegration of the p-nuclei 92Mo and 144Sm in the astrophysically relevant energy window: Proceedings of Science
Permalink: https://www.hzdr.de/publications/Publ-13300
Application of Focused Ion and Electron Beams in Materials Research
Bischoff, L.
Abstract
At the beginning the lecture I will briefly give an overview about the organization of the Research Centre Dresden-Rossendorf with different Institutes and research topics. In the Institute of Ion Beam Physics and Materials Research the application of ion beams in advanced materials science is manifold: for example, they are used to generate new or improved functional surfaces, and they are ideally suited to produce micro- and nanostructures in semiconductors. For these purposes in the Institute a couple of modern ion beam instruments for the fabrication and analysis of nanostructures is available. Among them there are a mass separated focused ion beam (FIB) and a crossbeam system, consisting of a high resolution Ga-FIB and a scanning electron microscope (SEM), which will be discussed more in detail. During the last decades, focused ion beams became a very useful and versatile tool in microelectronics industry, as well as in the field of basic and applied research and became an indispensable tool in nanotechnology. For special purposes like ion milling, ion beam writing for doping or patterning on μm- and nm-scale without any lithographic steps Ga+ and increasingly other ion species are of great interest. An introduction in design and operation of mass separated FIB systems (e.g. CANION31Mplus), equipped with metal alloy liquid ion sources as well as the development and characterization of them will be given. The combination of a focused electron beam with a high resolution FIB column in a crossbeam arrangement (NVision40) enables the in-situ inspection and analysis of FIB fabricated nanostructures with a resolution down to one nm without surface damaging. An included gas injection system allows the MO-CVD of nanostructures of different materials using either the focused ion or the electron beam. The fabrication possibilities of nanostructures, like nanowires, nanobridges and nanocantilevers by ion beam synthesis using different kinds of focused ion beams will be demonstrated and possible applications will be mentioned. Some examples, like ion beam synthesis of CoSi2 nano-structures, the generation of fluorescent colour centres, sputtering investigations and applications, the formation of ripples under FIB irradiation or the fabrication of NEMS structures on SOI substrates will be shown to demonstrate the manifold utilization of the microbeam technology. Furthermore, the possibility of varying the flux in the FIB by changing the pixel dwell-time in a wide range gives the opportunity to investigate radiation damage and dynamic annealing effects in Si, Ge, SiC and other materials at elevated implantation temperatures using different projectile ion species. Finally, the state-of art of FIB applications for TEM lamella preparation, FIB lithography of thin films and ion beam microscopy will be presented and shortly discussed.
Keywords: Focused Ion Beam; Liquid Metal Ion Source; Electron Microscopy; Nanotechnology
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Invited lecture (Conferences)
imdea nanociencia, 04.11.2009, Madrid, Spanien -
Invited lecture (Conferences)
Kolloquiumsvortrag, 10.12.2009, Leipzig, Deutschland
Permalink: https://www.hzdr.de/publications/Publ-13299
Pipe dream
Azzopardi, B.; Hampel, U.; Hunt, A.
Abstract
Gas-liquid flows are central to oil and gas production and because of the very flexible nature of the interface between the fluids, the flows can be very complex exhibiting a wide variety of three dimensional structures. In the field the steel pipes in which these two-phase mixture flow make it difficult to observe them. Even in the laboratory where pipes can be made of transparent plastic, we can still normally only see what is occurring near the pipe wall as bubbles clustering near the wall, or wavy films of liquid flowing along the walls, obscure what is occurring at the middle of the pipe. One way in which these visual limitations can be overcome is to employ electrical tomography methods. In research at the University of Nottingham we are working with Forschungzentrum Rossendorf-Dresden from Germany and Tomoflow Limited to use electrical tomography to 'see' into the pipe.
Keywords: multi-phase flow; wire mesh sensors; electrical capacitance tomography
- TCE - The chemical engineer (2009)820, 39-41
Permalink: https://www.hzdr.de/publications/Publ-13298
Simulating Strongly Coupled Plasmas on High-Performance Computers
Bussmann, M.; Schramm, U.; Thirolf, P.; Habs, D.
Abstract
Simulating strongly coupled plasmas is a demanding computational task. When a plasma is strongly coupled, the mutual Coulomb energy between the plasma particles is much stronger than their kinetic energy. Such a system can undergo a phase transition into a state in which long-range ordering of the plasma constituents can be observed. In a realistic simulation of the plasma dynamics one has to compute the total mutual interaction of each particle with each other particle for particle numbers up to hundred thousand particles. To study the microscopic and macroscopic dynamics of the plasma on a long time scale one thus has to rely on the computational power which is only available at supercomputing centers such as the Leibniz Rechenzentrum.
Keywords: strong coupling; plasma; ocp; one-component plasma; simulation; molecular dynamics; checker-board algorithm; laser cooling; particle; highly-charged ion; hci; cooling; stopping
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Contribution to proceedings
HLRB, KONWIHR and Linux-Cluster Review and Results Workshop, 08.-09.12.2009, Garching, Germany
Permalink: https://www.hzdr.de/publications/Publ-13297
GPU-based Particle-in-Cell Simulation
Burau, H.; Bussmann, M.; Schramm, U.; Cowan, T.; Widera, R.; Hönig, W.; Juckeland, G.
Abstract
Accelerating Plasma Simulations using novel computing hardware is a promising way towards a cost-efficient decrease of the runtime of realistic plasma simulations. We present a new particle-in-cell algorithm for simulating laser plasma acceleration of particles which has been developed to run on a NVIDIA GPU system. Using a sliding-window technique we are able to run large-scale 2D simulations of laser wakefield acceleration. We present the algorithm in detail and show that it is easy to extend to 3D geometries. We will conclude by discussing both obstacles and promises encountered when porting the algorithm to a standard CPU-based Linux cluster in which each node is equipped with one or more GPUs.
Keywords: gpu; gpgpu; cuda; particle-in-cell; pic; simulation; algorithm; cluster; message passing interface; pic; vampir; laser; plasma; acceleration
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Poster
ICNSP 09 - 21st International Conference on Numerical Simulation of Plasmas 2009, 06.-09.10.2009, Lisboa, Portugal
Permalink: https://www.hzdr.de/publications/Publ-13296
The economy of Yb:lasers
Siebold, M.
Abstract
Introduction of high-energy class diode-pumped solid-state lasers (HEC-DPSSLs) worldwide, efficiency limitations and energy extraction issues of high-energy laser based on Yb-doped materials, room-temperature vs. cryogenically cooled lasers, simulation and experimental results obtained with multi-pass pumping - a technique for efficiency enhancement.
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Lecture (others)
workshop on High-Energy Class Diode-Pumped Solid-State Lasers (HEC-DPSSL), 10.-12.06.2009, Dresden, Deutschland
Permalink: https://www.hzdr.de/publications/Publ-13295
Neue Materialien für Hochintensitätslaser sowie deren Anwendungen
Siebold, M.
Abstract
Erzeugung hoher Lichtintensitäten mittels Ultrakurzpulslaser, Laser-Teilchenbeschleunigung, diodengepumpte Festkörperlaser, neue Ytterbium-dotierte Lasermaterialien für Kurzpulslaserverstärker
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Invited lecture (Conferences)
workshop: Festkörperlaser Materialien und Anwendungen, 10.-11.09.2009, Berlin, Deutschland
Permalink: https://www.hzdr.de/publications/Publ-13294
Diode-pumped chirped pulse amplification to the TW level using Yb:CaF2
Siebold, M.; Hornung, M.; Hein, J.; Uecker, R.; Debus, A.; Kaluza, M. C.
Abstract
We present a terawatt diode-pumped chirped pulse amplifier using single-crystalline Yb:CaF2 as the gain medium. A maximum pulse energy of 420 mJ and a repetition rate of 1 Hz was obtained. After recompression, a pulse energy of 197 mJ and a pulse duration of 192 fs were achieved, corresponding to a peak power of 1TW.
Keywords: Diode-pumped lasers; Ytterbium-doped solid state lasers; optical pulse generation and pulse compression
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Contribution to proceedings
Ultra-Intense Laser Interaction Science (ULIS), 24.-29.05.2009, Frascati, Italia
Diode-pumped chirped pulse amplification to the TW level using Yb:CaF2, vol. 2109: American Institute of Physics, 119-122 -
Poster
Ultra-Intense Laser Interaction Science, 26.05.2009, Frascati, Italia
Permalink: https://www.hzdr.de/publications/Publ-13293
In-situ observation of secondary phase formation in Fe implanted GaN annealed in low pressure N-2 atmosphere
Talut, G.; Grenzer, J.; Reuther, H.; Shalimov, A.; Baehtz, C.; Novikov, D.; Walz, B.
Abstract
The formation of secondary phases in Fe implanted GaN upon annealing in low pressure N2-atmosphere was detected by means of in-situ x-ray diffraction and confirmed by magnetization measurements. A repeatable phase change from Fe2N at room temperature and Fe(3-x)N at 1023 K was observed in-situ. The phase transformation is explained by the change of lattice site and concentration of nitrogen within nitrides. The diffusion of Fe towards sample surface and oxidation with increasing annealing cycles limits the availability of secondary phase and hence the repeatability. At high temperature GaN dissolves and Ga as well as Fe oxidize due to presence of residual oxygen in the process gas. The ferromagnetism in the samples is related to nanometer sized interacting Fe(3-x)N crystallites.
Keywords: GaN; Fe-nitrides; DMS
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Applied Physics Letters 95(2009), 232506-1-232506-3
DOI: 10.1063/1.3271828
Cited 3 times in Scopus
Permalink: https://www.hzdr.de/publications/Publ-13292
Xe ion beam induced ripple structures on differently oriented single-crystalline Si surfaces
Hanisch, A.; Biermanns, A.; Pietsch, U.; Grenzer, J.; Facsko, S.
Abstract
We report on Xe+ induced ripple formation at medium-energy on single crystalline silicon surfaces of different orientation using substrates with an intentional miscut from the [001] direction and a [111] oriented wafer. The ion beam incidence angle in respect to the surface normal was kept fixed at 65° and the ion beam projection was parallel or perpendicular to the [110] direction. By a combination of atomic force microscopy, X-ray diffraction and high resolution transmission electron microscopy we found that the features of surface and the subsurface rippled structures such as ripple wavelength and amplitude and the degree of order do not depend on the surface orientation as assumed in recent models of pattern formation for semiconductor surfaces.
Keywords: ripples nanostructures Xe self-organisation silicon miscut ion implantation
- Journal of Physics D: Applied Physics 43(2010)11, 112001
Permalink: https://www.hzdr.de/publications/Publ-13291
Bestimmung des Ausdampfverhaltens des Reaktorkerns bei Ausfall der Nachkühlung im Mitte-Loop-Betrieb bei geöffnetem Reaktordeckel auf Basis von Rechnungen mit dem Programm ATHLET
Kliem, S.
Abstract
Unter Verwendung des Rechenprogramms ATHLET wurde das Ausdampfverhalten des Reaktorkerns bei Ausfall der Nachkühlung untersucht. Dafür wurde der Primärkreislauf des Reaktors vom Austritt aus dem Pumpenbogen bis zum Eintritt in den Dampferzeuger modelliert. Bei einer fest vorgegebenen Nachzerfallsleistung von 22 MW wurde das axiale Profil variiert. Neben einem symmetrischen kosinusähnlichen Profil wurden jeweils ein Profil für den Beginn und das Ende eines Brennstoffzyklus eines typischen Druckwasserreaktorkerns verwendet.
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Article, self-published (no contribution to HZDR-Annual report)
Forschungszentrum Rossendorf 2009
FZD\FWS\2009\06
26 Seiten
ISSN: 1437-322X
Permalink: https://www.hzdr.de/publications/Publ-13290
Characterization and tuning of ultrahigh gradient permanent magnet quadrupoles
Becker, S.; Bussmann, M.; Raith, S.; Fuchs, M.; Weingartner, R.; Kunz, P.; Lauth, W.; Schramm, U.; Ghazaly, M. E.; Grüner, F.; Backe, H.; Habs, D.
Abstract
The application of quadrupole devices with high field gradients and small apertures requires precise control over higher order multipole field components. We present a new scheme for performance control and tuning; which allows the illumination of most of the quadrupole device aperture because of the reduction of higher order field components. Consequently, the size of the aperture can be minimized to match the beam size achieving field gradients of up to 500 T m -1 at good imaging quality. The characterization method based on a Hall probe measurement and a Fourier analysis was confirmed using the high quality electron beam at the Mainz Microtron MAMI.
Keywords: compact; permanent; magnetic; quadrupole; lens; beam focusing; multipole; tuning; halbach; electron beam; x-fel
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Physical Review Accelerators and Beams 12(2009)10, 102801
DOI: 10.1103/PhysRevSTAB.12.102801
Permalink: https://www.hzdr.de/publications/Publ-13289
Measurement of Radiation Hardness of PET Components
Fiedler, F.; Braess, H.; Enghardt, W.
Abstract
In-beam PET has given valuable feedback on treatment quality over the 11 years of operation time between 1997 and 2008 of the heavy ion treatment facility at the Gesellschaft für Schwerionenforschung (GSI) Darmstadt. Based on this technical expertise a next generation of in-beam PET scanners will be developed. An experiment addressing the question whether the detectors and electronic components used in state-of-the-art PET-systems can be also utilized to configure a future in-beam PET scanner was performed at the medical beam line of GSI. The equipment for a new in-beam PET scanner should be tested whether it will resist the fluence of secondaries arising from the patient treatment of about 5 years. A ^12C beam of an energy of E=430.10AMeV was stopped in a PMMA phantom. The primary particle fluence of this irradiation was equivalent to about 5300 patient fractions (3 GyE per fraction). The detectors were placed at several angles to simulate a higher secondary particle fluence, i.e. a longer time of usage. They have been exposed to a secondary particle fluence equivalent up to 13 years of usage in an in-beam PET scanner. The equipment was provided by CPS and tested before and after the experiment. No damage was found applying the standard test procedure. analyzing the detectors after the experiment.
Keywords: radiation hardness; in-beam PET; ion therapy
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Lecture (Conference)
2009 IEEE Nuclear Science Symposium and Medical Imaging Conference, 25.-31.10.2009, Orlando, USA -
Contribution to proceedings
2009 IEEE Nuclear Science Symposium and Medical Imaging Conference, 23.10.-01.11.2009, Orlando, USA
Conference Record
Permalink: https://www.hzdr.de/publications/Publ-13288
A FAIR equation of state
Schulze, R.; Kämpfer, B.
Keywords: QCD; equation of state; FAIR; quasiparticles
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Lecture (others)
Institutsinternes WIP-Seminar, 16.10.2009, Dresden-Rossendorf, Deutschland
Permalink: https://www.hzdr.de/publications/Publ-13287
Discrimination of thioarsenites and thioarsenates by x-ray absorption spectroscopy
Suess, E.; Scheinost, A. C.; Bostick, B. C.; Merkel, B. J.; Wallschlaeger, D.; Planer-Friedrich, B.
Abstract
Soluble arsenic−sulfur compounds play important roles in the biogeochemistry of arsenic in sulfidic waters but conflicting analytical evidence identifies them as either thioarsenates (= AsV−sulfur species) or thioarsenites (= AsIII−sulfur species). Here, we present the first characterization of thioarsenates (mono-, di-, and tetrathioarsenate) by X-ray absorption spectroscopy and demonstrate that their spectra are distinctly different from those of AsIII−sulfur species, as well as from arsenite and arsenate. The absorption near edge energy decreases in the order arsenate > thioarsenates > arsenite > AsIII−sulfur species, and individual thioarsenates differ by 1 eV per sulfur atom. Fitted AsV−S and AsV−O bond distances in thioarsenates (2.13−2.18 Å and 1.70 Å, respectively) are significantly shorter than the corresponding AsIII−S and AsIII−O bond distances in AsIII−S species (2.24−2.34 Å and 1.78 Å, respectively). Finally, we demonstrate that thioarsenates can be identified by principal component analysis in mixtures containing AsIII−sulfur species. This capability is used to study the spontaneous reduction of tetrathioarsenate to AsIII−sulfur species (possibly trithioarsenite) upon acidification from pH 9.5 to 2.8.
Keywords: Arsenic; speciation; thioarsenite; thioarsenate; EXAFS; XANES
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Analytical Chemistry 81(2009)20, 8318-8326
DOI: 10.1021/ac901094b
Cited 91 times in Scopus
Permalink: https://www.hzdr.de/publications/Publ-13286
System Solution for Particle Therapy PET
Shakirin, G.; Braess, H.; Fiedler, F.; Kunath, D.; Laube, K.; Parodi, K.; Priegnitz, M.; Enghardt, W.
Abstract
At present, positron emission tomography (PET) is the only available technique for an in-vivo, non-invasive monitoring of the dose delivery precision in highly conformal ion beam therapy. The successful exploitation of in-beam PET at the Gesellschaft fuer Schwerionenforschung (GSI), Darmstadt, Germany during the last decade and a rising number of built or planned proton and heavier ion therapy facilities worldwide makes the development of a particle therapy PET (PT-PET) system of the next generation reasonable. The in-beam PET installation at GSI is a double-head positron scanner with a very limited solid angle which results in severe artifacts in the reconstructed images and in a low counting statistics. Thus, it is highly desirable to have larger solid angle coverage for PT-PET scanners of the next generation. However, increasing the effective area of a scanner might be limited by several requirements for the equipment of a radiotherapy treatment unit. Possible solutions for a prospective PT-PET system as well as a methodology for the evaluation of concurrent designs of the scanner taking into account the requirements of a therapy facility are discussed in this paper.
Keywords: in-beam PET; particle therapy; PT-PET
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Poster
2009 IEEE Nuclear Science Symposium and Medical Imaging Conference, 24.10.-01.11.2009, Orlando, USA -
Contribution to proceedings
IEEE NSS MIC, 24.-31.10.2009, Orlando, USA
System Solution for Particle Therapy PET
Permalink: https://www.hzdr.de/publications/Publ-13285
Quark stars from lattice QCD
Schulze, R.; Kämpfer, B.
Abstract
At small net baryon densities ab initio lattice QCD provides valuable information on the finite-temperature equation of state of strongly interacting matter. Our phenomenological quasiparticle model provides a means to map such lattice results to regions relevant for future heavy-ion experiments at large baryon density; even the cool equation of state can be inferred to address the issue of quark stars. We report on (i) the side conditions (charge neutrality, beta equilibrium) in mapping latest lattice QCD results to large baryon density and (ii) scaling properties of emerging strange quark stars.
Keywords: QCD; quasiparticle model
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Lecture (Conference)
Dense Matter in Heavy-Ion collisions and Supernovae, 11.-13.10.2009, Prerow, Deutschland
Permalink: https://www.hzdr.de/publications/Publ-13284
Synthesis of new bifunctional chelators for conjugation to vector molecules for tumor targeting.
Heldt, J.-M.; Ruffani, A.; Zenker, M.; Walther, M.; Stephan, H.; Pietzsch, H.-J.; Steinbach, J.
Abstract
Problem:
The goal of this study is to prepare novel chelators suitable for conjugation to vector molecules which can be labeled by yttrium or copper in order to achieve high specific activities and to improve pharmacokinetics. In this context, new water soluble bifunctional DOTA- and bis(2-pyridylmethyl)triazacyclocyclononane (DMPTACN)-based chelators have been synthesized and conjugated to the monoclonal antibody Cetuximab which binds to HER2 of the epithelial growth factor receptor (EGFR) family which is over-expressed by various tumors.
Material and Method:
Both chelators have been conjugated to Cetuximab via thiourea-bridging. Radiolabeling of DOTA derivatives has been performed in aqueous ammonium acetate solution at r.t. using 86YCl3 or 90YCl3. Radiolabeling of DMPTACN conjugates with 64Cu was achieved in MES buffer solution at 50°C using 64CuCl2. The affinity of the bioconjugates towards EGFR was determined by ELISA.
Results:
The ELISA test showed that the affinity of the bioconjugates has decreased compared to native Cetuximab. A chelator/antibody molar ratio of 4 was achieved as determined by MALDI-TOF-MS for the DOTA-Cetuximab conjugate. Radiolabeling of DOTA-conjugates with 86Y and 90Y at 37°C requires optimization to improve radiochemical yield. DMPTACN-Cetuximab conjugates can be rapidly labeled with 64Cu under mild conditions in almost quantitative yield.
Conclusions:
DMPTACN- and DOTA-ligands are attractive bifunctional chelating agents which can be conjugated to vector molecules for PET-imaging and radiotherapy. In the near future, the work with the ligands investigated will be extended using the pre-labeling approach.
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Lecture (Conference)
Targeting and Imaging of the Tumor Microenvironment, 23.-26.09.2009, Berder island, France
Permalink: https://www.hzdr.de/publications/Publ-13283
Structure-activity relationship of radiocopper-labeled DMPTACN-Bombesin conjugates
Ruffani, A.; Stephan, H.; Bergmann, R.; Steinbach, J.; Gasser, G.; Spiccia, L.
Abstract
Aim:
Radiometal‐labeled peptide derivatives of bombesin are very interesting targeting vectors for certain types of cancer. Bombesin derivatives have shown very high selectivity and affinity to
G‐protein‐coupled gastrin‐releasing‐peptide‐receptor (GRPR), which is over‐expressed in a variety of tumors including breast‐, prostate‐ and pancreatic‐tumors. Consequently, the
application of radiolabeled bombesin‐analogs for both the diagnosis and therapy of such tumors is being intensively investigated. However, the development of chemically and radiolytically
stable compounds which can be easily radiolabeled presents significant challenges. We recently showed that bis(2‐pyridylmethyl)triazacyclocyclononane (DMPTACN) was a promising candidate
for radiocopper‐labeling. In this study we examine structure‐activity relationships for new [64Cu]DMPTACN bombesin derivatives including their biodistribution and pharmacokinetics in
prostate cancer (PC3) xenografted tumor mice.
Methods:
Stabilized bombesin derivatives β‐Ala‐β‐Ala‐[Cha13,Nle14]BBN(7‐14) and β‐homo‐Glu‐β‐Ala‐β‐Ala‐[Cha13, Nle14]BBN(7‐14) were conjugated to the N‐terminus with DMPTACN ligands containing either a carboxylate or phenylisothiocyanate pendant arm via amide coupling and thiourea‐bridging, respectively. Radiolabeling of DMPTACN‐BBN derivatives with 64Cu was performed in aqueous ammonium acetate solution (pH=6) at 50°C using [64Cu]CuCl2. The affinity of DMPTACN‐BBN derivatives for the GRPR was determined using a competitive displacement/binding assay in human prostate (PC3) cancer cells. Internalization data for the [64Cu]Cu‐DMPTACN bombesin derivatives were obtained in the same cell line. Partition coefficients of the radiocopper‐labeled complexes of the DMPTACN‐BBN derivatives were determined in a 1‐octanol/buffer system. Biodistribution studies were performed on Wistar rats and NMRI nu/nu mice bearing the human prostate tumor PC‐3. Tumor accumulation was evaluated with small animal PET.
Results:
Radiolabeling of DMPTACNBBN‐bioconjugates was achieved in 30 min, yielding >99% radiochemical purity and specific activity up to 30 GBq/μmol after HPLC. DMPTACN‐NCS derivatives could be rapidly labeled with 64Cu under mild conditions in almost quantitative yield. The DMPTACN‐BBN conjugates showed high affinity to the GRPR and high uptake in PC‐3 cells. PET studies on tumor‐bearing PC‐3 mice revealed an accumulation in the GRPR‐positive tissue. Clear visualization of the tumor tissue and noticeable delineation from healthy tissue was achieved.
Conclusion:
DMPTACN ligands are attractive chelates for the development of radiocopper pharmaceuticals featuring very high chemical and radiolytical stability. They can be effectively coupled to target‐oriented peptides, such as bombesin. However, many issues need to be resolved, including the metabolic stabilization of the peptides and the direct fixation of radiometalated conjugates in the tumor tissue. DMPTACN‐isothiocyanate was found to be rapidly and efficiently labeled with 64Cu. These features make it a promising candidate as a pre‐labeling building block for antibody and synthetic polymers.
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Lecture (Conference)
Annual Congress of the European Association of Nuclear Medicine (EANM´09), 10.-14.10.2009, Barcelona, Spain -
Abstract in refereed journal
European Journal of Nuclear Medicine and Molecular Imaging 36(2009)Suppl. 2, S207
DOI: 10.1007/s00259-009-1227-5
Permalink: https://www.hzdr.de/publications/Publ-13282
Synthesis and Metabolic Stability of 11C-Labelled SU11248 Derivative as Inhibitor of Tyrosine Kinases
Knieß, T.; Bergmann, R.; Steinbach, J.
Abstract
Aim:
SU11248 is a novel inhibitor of receptor tyrosine kinases (RTKs) targeting vascular endothelial growth factor (VEGF) and plated‐derived growth factor (PDGF) [1]. Due to the fact that RTKs are overexpressed in some tumour entities, they might be a suitable target for cancer imaging by positron emission tomography (PET). A tyrosine kinase inhibitor labelled with a positron emitting isotope could represent a useful tool for monitoring levels of RTKs in tumour tissue by giving valuable information for anti‐angiogenic therapy. For this purpose we synthesized a methoxy substituted derivative of SU11248 and performed the radiosynthesis with the PET radionuclide carbon‐11 to the corresponding 11C‐labelled radiotracer. First investigations on the in vivo metabolic stability of the new 11C‐labelled SU11248 derivative are reported.
Materials and methods:
The radiolabelling was performed via 11C‐methylation reaction of the corresponding desmethyl precursor with [11C]MeI in a TRACERLab FXC gas phase synthesizer (GE). After purification by semi‐preparative HPLC and solid phase extraction the radiotracer was dispensed with E153 electrolyte solution and injected intravenously into male Wistar rats. For metabolite analysis blood samples were taken from the arteria femoralis at 1.5; 3; 5; 10, 20, 30 and 60 minutes past injection. After centrifuging blood samples 5 min 13.000 rpm at 4°C plasma was analyzed by radio HPLC.
Results:
The synthesis of the non‐radioactive methoxy‐substituted SU11248 as well as the desmethyl precursor was accomplished by reacting 5‐methoxy‐ and 5‐hydroxyl‐oxindole with 5‐formyl‐2,4‐dimethyl‐1H‐pyrrole‐3‐carboxylic‐acid‐(2‐diethylaminoethyl)‐amide. Radiolabelling was achieved by reaction of the 5‐hydroxy‐substituted SU11248 derivative with [11C]CH3I in DMF/aqueous NaOH at 80°C. After semi‐preparative HPLC purification the 11C‐labelled radiotracer was obtained in 14‐17% decay corrected radiochemical yield at a specific activity of 162‐198 GBq/μmol at the end of synthesis in 94‐99% radiochemical purity. Metabolism analysis in rat plasma showed 96% of intact compound 3 min and 73% 60 min p.i., together with three more polar metabolites.
Conclusion:
The new 11C‐labelled derivative of SU11248 can be synthesized in good radiochemical yield, sufficient purity and high specific activity. The found metabolic stability in rat plasma showing 73% of intact radiotracer 60 min p.i. suggests that the 11C‐methoxy labelling group is preserved under in vivo conditions. These findings are encouraging for further investigation with this radiotracer on RTK expressing cells and tumour tissue to answer the question if this radiotracer would be a useful tool for monitoring angiogenic processes by PET. [1] Sun L., Liang C. et al., J. Med. Chem., 46, (2003), 1116
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Poster
Annual Congress of the European Association of Nuclear Medicine (EANM), 10.-14.10.2009, Barcelona, Spain -
Abstract in refereed journal
European Journal of Nuclear Medicine and Molecular Imaging 36(2009)Suppl. 2, S310-S311
DOI: 10.1007/s00259-009-1227-5
Permalink: https://www.hzdr.de/publications/Publ-13281
Structural Aspects of Uranyl Complexes with Lipopolysaccharide
Barkleit, A.; Li, B.; Foerstendorf, H.; Rossberg, A.; Moll, H.; Bernhard, G.
Abstract
It is well-known that microorganisms play an important role in bioremediation. Because of the high retention capability of heavy metal ions, they significantly influence mobilization and immobilization of cations in soils. The prediction of the radionuclide transport in the environment and the improvement of technical bioremediation strategies require a detailed understanding of the binding mechanisms on a molecular level.
Lipopolysaccharide (LPS), the main part of the outer membrane of Gram-negative bacteria, sticks out of the cell wall and is in direct contact with the (aqueous) environment. With its high content of negatively charged functional groups (mainly carboxyl and phosphoryl groups) it plays a key role in protection of contaminants.
We investigated the uranyl LPS interactions to gain detailed information about the coordination sphere in the molecular environment of the uranyl ion. We focused on the identification of the coordinating functional groups over a wide pH range (from 2.5 to 7) and under different stoichiometric conditions. In particular, the discrimination between carboxyl and phosphoryl groups and their binding behaviours was elucidated by extended X-ray absorption fine structure (EXAFS) spectroscopy at the U LIII-edge and attenuated total reflection Fourier-transform infrared (ATR FT-IR) spectroscopy. With respect to environmental conditions, samples with an excess of LPS were investigated by EXAFS. Furthermore, samples with equimolar ratios of uranyl and functional groups of LPS according to a slight deficit of phosphoryl groups were determined with FT-IR.
EXAFS spectra show great similarities to the uranyl mineral phase meta-autunite. A four-fold complexation of the uranium was derived from very short U Oeq distances of 2.28 Å and U P distances of 3.58 Å indicating unidentate coordinated phosphoryl groups. Furthermore, U U interactions can be observed at 5.2 Å and 6.9 Å.
FT-IR spectra show spectral evidence for both, carboxyl and phosphoryl coordination. A downshift of the antisymmetric stretching mode of the carboxylate group from 1576 (uncomplexed LPS) to 1530 cm−1 and an upshift of the symmetric stretching mode from 1404 (uncomplexed LPS) to 1455 cm−1 upon complexation provides evidence for a bidentate complexation to carboxylate groups. The antisymmetric and symmetric stretching modes of the complexing phosphoryl groups are observed at 1105 and 1060 cm−1.
In summary, we determined at high LPS excess preferential phosphoryl coordination, whereas with an increasing relative amount of uranyl ions, corresponding to a decreasing number of functional groups of LPS, additional carboxylate coordination becomes important. This complexation behaviour remains within a broad pH range from slight acidic to neutral values. Under the investigated experimental conditions, the coordination of uranyl ions to the LPS molecule is obviously controlled by the U/LPS concentration ratio irrespective from prevailing pH.
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Lecture (Conference)
RadChem 2010 - 16th Radiochemical Conference, 18.-23.04.2010, Marianske Lazne, Czech Republic
Permalink: https://www.hzdr.de/publications/Publ-13280
Investigations on seepage waters of the test site Gessenwiese by TRLFS
Baumann, N.; Arnold, T.
Abstract
The test field Gessenwiese was installed on a leaching heap at the former uranium mining area Ronneburg (western Thuringia) for investigations in acid mining drainage and in heavy metals retention, especially uranium (Grawunder A. et al. 2009). The uranium speciation in seepage water of the Gessenwiese was determined by TRLFS. Time-resolved laser-induced fluorescence spectroscopy (TRLFS) posses some superior features, above all a very high sensitivity for fluorescent heavy metal ions. The predominance of TRLFS compared to other spectroscopic techniques, e.g. XRD and IR was showed in Baumann N. et al. (2008) in analyzing the speciation of U(VI) in a thin layer of an alteration product formed on depleted uranium. TRLFS analyses in seepage water of the Gessenwiese were carried out to compare it in a later stage with the uranium speciation in plants, which grow on that grassland and may take up uranium contaminated water.
Grawunder A. et al. Chem Erde-Geochem. 69 5-19 (2009)
Baumann N. et al. Environ. Sci. Technol. 42 8266-8269 (2008)
Keywords: Uranium; Speciation; TRLFS
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Contribution to proceedings
16th Radiochemical Conference, 18.-23.04.10, Marienbad, Tschechische Republik
Chemické listy S - Booklet of Abstracts, Praha: CSAV, s190
Permalink: https://www.hzdr.de/publications/Publ-13279
Investigations on Stability and Structure of Thorium Colloids in near-neutral Solutions
Dreissig, I.; Weiss, S.; Zanker, H.; Hennig, C.; Brendler, E.; Bernhard, G.
Abstract
This work presents results about the formation of thorium(IV) colloids and precipitates in the presence of silicic acid. Three methods were used for the preparation of the thorium compounds:
- Experiment A: Silicic acid concentrations and ionic strengths were adjusted in the presence of preformed stable ThO2 colloids at neutral pH (0.4 mM Th; 0 3 mM Si; I = 0.05 M NaClO4)
- Experiment B: Precipitation of ThO2 colloids in the presence of silicic acid by neutralization from the acidic side of the pH scale (1 mM Th; 0-4.2 mM Si; I = 0.1 M NaClO4)
- Experiment C: Precipitation of Th(IV) colloids in the presence of silicic acid by neutralisation of a Th(IV) carbonate solution from the alkaline side of the pH scale (1 mM Th; 0-3 mM Si; I = 0.1 M NaClO4)
The zeta potentials of the thorium compounds in experiments A, B and C were determined by laser Doppler velocimetry at pH values of 2 10. These measurements allowed the estimation of the isoelectric points (IEPs) of the colloids and conclusions about the colloidal stability of the suspensions formed.
By the addition of silicic acid to preformed ThO2 colloids (experiment A), a significant shift of the IEPs from pH ~ 8.5 to lower values (pH ~ 6.5) was observed. Similar results were found in experiment B. Here, the IEP shifted from pH ~ 7.3 to pH ~ 6.0 in the presence of silicic acid. For both experiments the shift of the IEP was a function of the silicic acid concentration. Obviously, the significant amounts of silicate in/on the Th(IV) particles shift the IEP toward the IEP of pure silicic acid (pH < 3[1]).
On the other hand, the results of the zeta potential measurements on the Th(IV) colloids from experiment C demonstrated that the IEP did not change in the presence of varying amounts of silicic acid but remained constantly at pH ~ 5.2. It was also significantly lower than the IEPs of the colloids from experiments A and B formed under acidic conditions. The IEP behaviour of the experiment C colloids is not yet fully understood.
The results of 29Si solid state NMR and EXAFS spectroscopy of the thorium samples from experiment C showed that silicate was built in into the solid structure of ThO2. A possible mechanism is the partial replacement of the Th-O-Th bonds by bridging silicic acid and the formation of Th-O-Si-O-Th links. It is discussed whether the integration of silicic acid in the solid structure results in the formation of a still unknown thorium compound or a thorite (ThSiO4) like material was formed.
[1] R. K. Iler, K. Ralph, The Chemistry of Silica: Solubility, Polymerization, Colloid and Surface Properties and Biochemistry of Silica, John Wiley & Sons, 1979.
Keywords: Colloid; nanoparticle; zetapotential; isoelectric point; thorium; Th(IV); silicic acid; silicate; EXAFS; 29-Si-NMR
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Contribution to proceedings
RadChem 2010 - 16th Radiochemical Conference, 18.-23.04.2010, Marianske Lazne, Czech Republic
Radchem 2010 - BOOKLET OF ABSTRACTS CONFERENCE PROGRAMME
Permalink: https://www.hzdr.de/publications/Publ-13278
Effect of the Nature of Anions of Aluminum Salts Used to Synthesize a Precursor of the Al2O3-ZrO2 Ceramics on the Stabilization of the Tetragonal Modification of Zirconium Dioxide
Zharnylskaya, A. L.; Volkhin, V. V.; Reuther, H.
Abstract
Samples of a precursor for an aluminum oxide ceramics reinforced with zirconium oxide were synthesized by hydrolysis of various aluminum salts in the presence of a ZrO2 sol under conditions of urea decomposition at 90 degrees C and pH < 4 maintained, with hydrolysis products deposited onto the surface of ZrO2 sol particles. It was found that the nature of a salt anion affects the interaction of hydrolysis products of the aluminum cation with the surface of ZrO2 sol particles. The structure of products formed in thermal treatment of samples of a precursor for Al2O3-ZrO2 (T = 1250 degrees C) was characterized by X-ray phase analysis and scanning electron microscopy. The phase transition temperatures of the oxides Al2O3 and ZrO2 contained in the precursor were estimated using the results of thermal analysis of the samples in the temperature range 20-1300 degrees C.
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Russian Journal of Applied Chemistry 82(2009), 1364-1369
DOI: 10.1134/S1070427209080084
ISSN: 1070-4272
Cited 2 times in Scopus - Zurnal prikladnoj chimii 82(2009), 1268-1272
Permalink: https://www.hzdr.de/publications/Publ-13277
Improvement of Satellite Imaging Câmera Components Made of SS304 by Nitrogen PIII Treatments
Siqueira, R. H. M.; Ueda, M.; Lepienski, C. M.; Reuther, H.
Abstract
Improvement of Satellite Imaging Câmera Components Made of SS304 by Nitrogen PIII Treatments
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Poster
10th International Workshop on Plasma Based Ion Implantation and Deposition, 07.-11.09.2009, São José dos Campos, Brasil
Permalink: https://www.hzdr.de/publications/Publ-13276
Enhancement of Surface Properties of SAE 1070 by Chromium Plasma Immersion Ion Implantation and Deposition
Mello, C. B.; Ueda, M.; Oliveira, R. M.; Reuther, H.; Lepienski, C. M.
Abstract
Enhancement of Surface Properties of SAE 1070 by Chromium Plasma Immersion Ion Implantation and Deposition
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Lecture (Conference)
10th International Workshop on Plasma Based Ion Implantation and Deposition, 07.-11.09.2009, São José dos Campos, Brasil
Permalink: https://www.hzdr.de/publications/Publ-13275
Modificação da Superfície da Liga Ni-Ti Pela Implantação Iônica por Imersão em Plasma
Camargo, E. N.; Silva, M. M.; Baldissera, S.; Ueda, M.; Otubo, J.; Reuther, H.
Abstract
Modificação da Superfície da Liga Ni-Ti Pela Implantação Iônica por Imersão em Plasma
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Lecture (Conference)
64º Congresso da ABM Associação Brasileira de Metalurgia, Materiais e Mineração, 13.-17.07.2009, Expominas, Belo Horizonte, Brasil
Permalink: https://www.hzdr.de/publications/Publ-13274
Characteristics of Austenitic Stainless Steel Nitrided in a Hybrid Glow Discharge Plasma
Oliveira, R. M.; Ueda, M.; Silva, L. L. G.; Reuther, H.; Lepienski, C. M.
Abstract
Characteristics of Austenitic Stainless Steel Nitrided in a Hybrid Glow Discharge Plasma
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Brazilian Journal of Physics 39(2009), 554-558
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Lecture (Conference)
17th International Conference on Wear of Materials, 19.-23.04.2009, Las Vegas, USA
Permalink: https://www.hzdr.de/publications/Publ-13273
Nanoindentation response and microstructure of irradiated Fe-Cr alloys
Bergner, F.; Heintze, C.; Hernandez-Mayoral, M.
Abstract
Self-ion irradiation in combination with nanoindentation offers the possibility to characterize irradiation damage in a broad range of irradiation temperature and fluence. Nanoindentation results are reported for Fe-Cr alloys containing 2.5 to 12.5 at% Cr irradiated at ambient and elevated temperatures. The investigation also comprises dual-beam ion irradiations. The effects of indentation load, Cr content, fluence and irradiation temperature are discussed. We have found cases of both broad consistence with and deviations from reported trends. Hardening features are characterized by means of TEM. The results are compared with TEM, SANS and hardness data reported for neutron-irradiated conditions of the same alloys.
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Lecture (Conference)
IAEA Technical Meeting on Physics of Materials under Neutron and Charged Particle Irradiation, 16.-19.11.2009, Wien, Österreich
Permalink: https://www.hzdr.de/publications/Publ-13272
FP7 project LONGLIFE: Treatment of long term irradiation embrittlement effects in RPV safety assessment
Altstadt, E.; Bergner, F.; Hein, H.; Gillemot, F.; Serrano, M.; Brumovsky, M.; Lidbury, D.; Marcelles, I.
Abstract
In view of the increasing age of the European NPPs and envisaged life time extensions up to an EOL of 80 years, there is a need for an improved understanding of RPV irradiation embrittlement effects specific to long term operation (LTO). The project aims at: 1) improved knowledge on LTO phenomena relevant for European reactors; 2) assessment of prediction tools, codes, standards and surveillance guidelines. The scope of work comprises the analysis of LTO boundary conditions, microstructural investigations (e.g. LBP) and supplementary mechanical tests (e.g. RPV steels from decommissioned plants), training activities and elaboration of recommendations for RPV materials assessment and embrittlement surveillance under LTO conditions. The duration of the collaborative project will be 36 months with 15 partners participating.
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Invited lecture (Conferences)
15th Workshop of the International Group on Radiation Damage Mechanisms in Pressure Vessel Steels (IGRDM-15), 11.-16.10.2009, Budapest, Ungarn
Permalink: https://www.hzdr.de/publications/Publ-13271
Fluence dependence of SANS and yield stress increase observed for low-Cu RPV steels
Bergner, F.; Ulbricht, A.; Viehrig, H.-W.
Abstract
The investigation is focussed on three low-Cu RPV steels, JPB, JPC and JFL, irradiated at 255°C up to several levels of neutron fluence. The SANS data obtained will be discussed as a function of fluence and correlated with measured values of the yield stress increase. There is strong evidence for a late-blooming effect from both SANS and hardening. The results will be compared with those from similar investigations for RPV steels and model alloys irradiated at higher temperatures and higher flux.
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Lecture (Conference)
15th Workshop of the International Group on Radiation Damage Mechanisms of Pressure Vessel Steels (IGRDM-15), 11.-16.10.2009, Budapest, Ungarn
Permalink: https://www.hzdr.de/publications/Publ-13270
The microstructure of neutron-irradiated Fe-Cr alloys: A small-angle neutron scattering study
Bergner, F.; Heintze, C.; Ulbricht, A.
Abstract
Ferritic-martensitic chromium steels are candidate materials for future applications in both Gen-IV fission and fusion technology. Experimental investigation of neutron-irradiated Fe-Cr model alloys is important in order to gain a better understanding of the interplay of chromium content and irradiation behaviour. Small-angle neutron scattering (SANS) is particularly well suited to unfold the size distribution of non-planar irradiation-induced nanoscale features such as defect-solute clusters, nanovoids and -particles. This size distribution represents a statistically reliable average over a macroscopic volume. Assumptions on the dominant type of features can be checked against the ratio of magnetic and nuclear scattering.
The materials investigated in this work are commercial-purity Fe-Cr alloys of nominal compositions Fe-2.5Cr, Fe-5Cr, Fe-9Cr and Fe-12.5Cr (at%). Neutron irradiation was performed in the reactor BR2 at Mol (Belgium) at a temperature of 300°C and neutron flux of 9 x 1013 cm-2 s-1 (E > 1 MeV) [Matijasevic, JNM 377 (2008) 147]. The neutron exposures expressed in units of displacements per atom correspond to 0.6 and 1.5 dpa. A wavelength of 0.58 nm and three detector-sample distances of 1, 4 and 16 m were used in the SANS experiments carried out at the SANS-2 facility of GKSS Geesthacht (Germany). The samples were placed in a saturation magnetic field in order to separate magnetic and nuclear contributions. The scattering curves obtained for the unirradiated conditions of the four Fe-Cr alloys were taken as reference.
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Lecture (Conference)
Joint EC-IAEA Topical Meeting on Development of New Structural Materials for Advanced Fission and Fusion Reactor Systems, 05.-09.10.2009, Barcelona, Spanien
Permalink: https://www.hzdr.de/publications/Publ-13269
Characterization of Fe-Cr alloys using SANS, nanoindentation and ultrasound
Heintze, C.; Bergner, F.; Ulbricht, A.
Abstract
Ferritic/martensitic Cr-steels are candidate structural materials for future nuclear applications. Fe-Cr alloys serve as model alloys for the investigation of the effect of Cr on microstructure, properties and irradiation behaviour. Industrial purity Fe-Cr alloys of Cr levels of 2.5, 5, 9 and 12 at% were produced at SCKCEN Mol within the MIRE project and characterized with respect to composition, microstructure, dislocation arrangement and tensile properties [M. Matijasevic et al., JNM 377 (2008) 147]. The present contribution is devoted to the complementary characterization of the same set of materials by means of small angle neutron scattering (SANS), depth-sensing nanoindentation and sound velocity measurements.
SANS experiments were performed in the wide range of scattering vectors from 0.03 to 3 nm 1 using three different sample-detector distances. Incoherent and coherent scattering were identified and discussed as a function of Cr content. Depth-sensing nanoindentation was performed at maximum loads ranging from 1 to 500 mN and supplemented with Vickers hardness. Interestingly, some of the curves representing the load dependence of nanohardness for different Cr contents cross one another indicating an effect of Cr on the indentation-size effect. The velocity of both longitudinal and shear waves was measured using the ultrasound pulse-echo technique. The polycrystalline averages of the elastic constants were estimated as a function of Cr. First results on the effect of both ion and neutron irradiation will also be presented.
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Lecture (Conference)
EUROMAT 2009, 07.-10.09.2009, Glasgow, United Kingdom
Permalink: https://www.hzdr.de/publications/Publ-13268
Cluster dynamics simulation of point defect clusters in neutron irradiated pure iron
Gokhman, A.; Bergner, F.
Abstract
The effect of the size dependence of production rate of point defect clusters is taken into account in the cluster dynamics modeling of the simultaneous formation of vacancy clusters and self-interstitial atom clusters in neutron irradiated pure iron. The calibration of material parameters has been carried out. The correspondence between small angle neutron scattering, transmission electron microscopy and positron annihilation spectroscopy and cluster dynamics data is studied.
Keywords: Neutron irradiation; Pure iron; Cluster dynamics (CD)
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Radiation Effects and Defects in Solids 165(2010), 216-226
DOI: 10.1080/10420151003631928
ISSN: 1042-0150
Cited 29 times in Scopus
Permalink: https://www.hzdr.de/publications/Publ-13267
Arsenic doped p-type zinc oxide films grown by radio frequency magnetron sputtering
Fan, J. C.; Zhu, C. Y.; Fung, S.; Zhong, Y. C.; Wong, K. S.; Xie, Z.; Brauer, G.; Anwand, W.; Skorupa, W.; To, C. T.; Yang, B.; Beling, C. D.; Ling, C. C.
Abstract
As-doped ZnO films were grown by the radio frequency magnetron sputtering method As the substrate temperature during growth was raised above ~400°C, the films changed from n-type to p-type. Hole concentration and mobility of ~6x10^17 cm^-3 and ~6 cm^2 V^-1 s^-1were achieved. The ZnO films were studied by secondary mass spectroscopy, x-ray photoelectron spectroscopy (XPS), low temperature photoluminescence (PL), and positron annihilation spectroscopy (PAS). The results were consistent with the As/Zn-2V/Zn shallow acceptor model proposed by Limpijumnong et al. [Phys. Rev. Lett. 92 155504 (2004)]. The results of the XPS, PL, PAS, and thermal studies lead us to suggest a comprehensive picture of As-related shallow acceptor formation.
Involved research facilities
- P-ELBE
- Journal of Applied Physics 106(2009), 073709-1-073709-6
Permalink: https://www.hzdr.de/publications/Publ-13266
Hydrodynamische Untersuchungen in Festbettreaktoren mit Gittersensoren
Schubert, M.
Abstract
Kenntnisse über die Gas/Flüssig-Strömungen in chemischen Reaktoren und Kolonnen sind von elementarer Bedeutung für die Auslegung und den effizienten Betrieb. Besonders bei der Durchströmung von Schüttungen und Packungen könnten Fehlverteilungen auftreten und damit Druckverlust und Ausbeute nachteilig beeinflussen. Die am Forschungszentrum Dresden-Rossendorf entwickelten Gittersensoren stellen eine hybride Messtechnik dar, die die Vorteiler lokalen Sonden und tomographischer Verfahren kombiniert. In porösen Packungen können Flüssigkeitsanteile und Flüssigkeitsgeschwindigkeiten mit hoher zeitlicher Auflösung im Durchströmungsquerschnitt verteilt ermittelt werden.
Der Vortrag gibt eine Übersicht zu Anwendung und Untersuchungsmöglichkeiten von Gas/Flüssig-Strömungen in Packungen mit den Schwerpunkten Strömungsvisualisierung, Holdupverteilung und Geschwindigkeitsmessung. Exemplarisch wird die Anwendung der Gittersensoren für größere Reaktordurchmesser demonstriert.
Keywords: wire mesh sensors; liquid holdup; liquid velocity; industrial scale sensor
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Lecture (others)
Seminar "Sensoranwendung in der Chemieindustrie" der BASF Ludwigshafen, 14.10.2009, Ludwigshafen, Germany
Permalink: https://www.hzdr.de/publications/Publ-13265
Spatially resolved inline measurement of liquid velocity in trickle bed reactors
Schubert, M.; Khetan, A.; Da Silva, M. J.; Kryk, H.
Abstract
The flow pattern in trickle bed reactors is of an inhomogeneous nature due to a random packing structure. Thus, the local values for liquid phase ratio and velocity are spread over the whole cross-section and a global determination of these values ignores the fact that local phenomena dominate mass and heat transfer and eventually the reactor efficiency. Only if both parameters can be locally quantified, can a realistic picture of the flow fields be drawn.
A new wire-mesh sensor (WMS) setup based on the measurement of electrical permittivity of fluids was used, which can be applied to the packings of porous catalyst particles. A calibration method is proposed to get access to the liquid saturation. Axial velocity distributions are measured via a method based on the spatial tracer pulse time-of-flight between sensing points of two WMSs installed at a distance of few millimeters. The effects of gas and liquid flow rates on local liquid velocities were analyzed.
The proposed technique was validated against liquid collector data, which showed very good agreement. For this purpose, distributions of the volumetric flow rate were calculated by applying the continuity equation to the saturation and velocity data obtained from WMS.
Keywords: Capacitance wire-mesh sensor; Trickle bed reactor; Local liquid velocity; Liquid saturation
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Chemical Engineering Journal 158(2010)3, 623-632
DOI: 10.1016/j.cej.2010.02.009
Cited 34 times in Scopus
Permalink: https://www.hzdr.de/publications/Publ-13264
Co-current descending two-phase flows in inclined packed beds: experiment versus simulations
Atta, A.; Schubert, M.; Nigam, K. D. P.; Roy, S.; Larachi, F.
Abstract
The effect of inclination angle of a packed bed on its corresponding gas-liquid flow segregation and liquid saturation spatial distribution was measured in co-current descending gas-liquid flows for varying inclinations and fluid velocities, and simulated using a two-phase Eulerian computational fluid dynamics framework (CFD) adapted from trickle-bed vertical configuration and based on the porous media concept. The model predictions were validated with our own experimental data obtained using electrical capacitance tomography. This preliminary attempt to forecast the hydrodynamics in inclined packed bed geometries recommends for the formulation of appropriate drag force closures which should be integrated in the CFD model for improved quantitative estimation.
Keywords: Inclined packed bed; Hydrodynamics; Two-phase segregated flow; Multiphase flow visualization; Electrical capacitance tomography; Computational fluid dynamics
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Canadian Journal of Chemical Engeneering 88(2010)5, 742-750
DOI: 10.1002/cjce.20340
Cited 28 times in Scopus
Permalink: https://www.hzdr.de/publications/Publ-13263
Hydrodynamics of co-current two-phase flows in slanted porous media - modulation of pulse flow via bed obliquity
Schubert, M.; Hamidipour, M.; Duchesne, C.; Larachi, F.
Abstract
A packed bed operated with descending gas-liquid co-current flows in slanted configuration to force trickle flow pattern to segregate due to gravity was studied, in addition to dependences to inclination angle of liquid saturation and pressure drop. Inception of pulse flow regime could take place regardless of inclination angle and the transition from segregated/trickle regime to pulse flow regime was experimentally determined. The Grosser et al.1 flow regime transition model was modified by considering only axial components of the gas and liquid superficial velocities to predict the slant-dependent shifts in transition from segregated/trickle to pulse flow and was found to agree with experimental data. Pulse flow regime at different inclinations was characterized with respect to frequency, velocity and shape of pulses. Bed obliquity was unveiled as a new artifice to pulse flow modulation with possible prospects for catalytic reactions requiring antagonistically high-interaction regime mass transfer coefficients and partial catalyst wetting.
Keywords: Packed bed hydrodynamics; inclination; segregation; electrical capacitance tomography; flow regime transition; transition model
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AIChE Journal 56(2010)12, 3189-3205
DOI: 10.1002/aic.12237
Cited 40 times in Scopus
Permalink: https://www.hzdr.de/publications/Publ-13262
KKW Krümmel: Spannungs- und Ermüdungsanalyse des Kernmantels für die Transiente am 28.06.2007
Altstadt, E.; Werner, M.
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Article, self-published (no contribution to HZDR-Annual report)
Forschungszentrum Rossendorf 2008
FZD\FWS\2008\09
20 Seiten
ISSN: 1437-322X
Permalink: https://www.hzdr.de/publications/Publ-13261
Dynamics of Mesoscopic Magnetic Objects
Quitmann, C.; Raabe, J.; Puzic, A.; Kuepper, K.; Wintz, S.
Abstract
We report on the dynamic properties of mesoscopic magnetic objects. Such objects have dimensions somewhat larger than the magnetic exchange length ξ. This leads to relatively simple and stable patterns of the magnetization which can be excited using magnetic field pulses. The subsequent dynamics can be studied using x-ray based magnetic microscopy. We show examples of high symmetry structures where the dynamics is relatively simple and can be analyzed quantitatively in terms of amplitude, frequency, damping and symmetry. Intentional defects allow modifying specific modes. When using high amplitude excitations the magnetization in such structures can be switched.
Keywords: magnetism; dynamics; vortex; XMCD
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Contribution to external collection
Beaurepaire, E.; Bulou, H.; Scheurer, F.; Kappler, J.-P.: Magnetism and Synchrotron Radiation - New Trends; Springer Proceedings in Physics, Vol. 133, Berlin, Heidelberg: Springer, 2010, 978-3-642-04497-7
Permalink: https://www.hzdr.de/publications/Publ-13260
Implantation, Diffusion, Activation, and Recrystallization of Gallium Implanted in Preamorphized and Crystalline Germanium
Hellings, G.; Wündisch, C.; Eneman, G.; Simoen, E.; Clarysse, T.; Meuris, M.; Vandervorst, W.; Posselt, M.; de Meyer, K.
Abstract
We investigated the as-implanted profiles, electrical activation, diffusion, and recrystallization of gallium implanted in germanium samples through the combination of secondary-ion mass spectrometry, transmission electron microscopy, and sheet resistance measurement. Because of their high activation level (4.4 x 1020 cm−3) without preamorphization, low activation temperature (400°C), and absence of diffusion (up to 700°C), Ga junctions in crystalline Ge are very promising candidates for implementation in germanium technology. In the amorphous Ge phase, an increased diffusivity of Ga was observed at temperatures above 400°C.
Keywords: germanium gallium diffusion activation recrystallization
- Electrochemical and Solid State Letters 12(2009), H417-H419
Permalink: https://www.hzdr.de/publications/Publ-13259
Millisecond flash lamp annealing of ultra-shallow implanted layers in Ge
Posselt, M.; Wündisch, C.; Schmidt, B.; Schumann, T.; Mücklich, A.; Skorupa, W.; Clarysse, T.; Simoen, E.; Hortenbach, H.
Abstract
In the past the lack of a stable native germanium oxide for surface passivation and gate dielectrics as well as the inability to epitaxially grow sufficiently thick defect-free germanium layers on silicon hindered the integration of germanium into the mainstream Si-based technology. Recent developments, such as high-k dielectrics and germanium-on-insulator substrates have made germanium a promising candidate for future high-mobility and low-power consumption devices. Therefore, electrical doping of germanium by ion implantation and subsequent annealing has drawn a renewed interest. Investigations on the formation of ultra shallow junctions by ion beam processing have shown that p+-doping using B yields junctions that meet the requirements for the 22 nm technology node, whereas the formation of n+-junctions by P or As is complicated by the high diffusivity and the low solubility of the dopants. Recently, the concentration-dependent diffusion of n-dopants like P, As and Sb has been explored, and it has been found that doubly negatively charged vacancies are the mobile species responsible for the migration of the dopant atoms. The application of conventional rapid thermal annealing (RTA) with durations of some seconds and temperatures above about 500 °C leads to the activation of the n-dopants but their fast concentration-dependent diffusion can generally be not prevented. On the other hand it has been shown that both the diffusion and the activation of the dopants does not depend significantly on the implantation damage, i.e. using the defect engineering schemes known from Si technology seems to be not promising. Therefore, in order to control junction depth and dopant activation ultra-short annealing by flash lamps or lasers are currently under investigation.
The present work deals with the application of millisecond flash lamp annealing (FLA) to samples containing an implanted surface layer of about 100 nm thickness. P or As ions were implanted at an energy of 30 or 90 keV, respectively, and a fluence of 3x1015 cm-2. The investigations are focused on solid phase recrystallization, dopant redistribution and dopant activation. The dependence of these effects on the heat transfer to the sample during FLA as well as on pre-amorphization and pre-annealing treatment is discussed. The results are compared to typical data achievable by RTA. Different characterization methods were employed. Channeling Rutherford backscattering spectrometry and cross-sectional transmission electron microscopy (XTEM) were used to monitor the recrystallization of the amorphous layers formed during implantation. The depth distributions of P and As were measured by secondary ion mass spectrometry. In order to determine the sheet resistance variable probe spacing and micro four point probe measurements were utilized. Selected samples were studied by XTEM to search for precipitates and end-of-range defects. While in RTA the concentration dependent dopant diffusion hinders the formation of ultra-shallow n+ layers, FLA does not cause any diffusion. The maximum activation obtained by FLA is about 4x1019 and 2x1019 cm-3 for P and As, respectively. This is about 3-4 times higher than under typical RTA conditions. However, the activation and the sheet resistance achieved by FLA do not yet fulfill the ITRS requirements for the 22 nm technology node. Possible mechanisms responsible for dopant deactivation are discussed.
Keywords: germanium flash lamp annealing ion implantation
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Invited lecture (Conferences)
216th Meeting of the Electrochemical Society, Symposium E10: ULSI Process Integration 6, 04.-09.10.2009, Vienna, Austria
Permalink: https://www.hzdr.de/publications/Publ-13258
Atomistic simulation of recrystallization of amorphous Si and Ge
Posselt, M.; Gabriel, A.
Abstract
Recrystallization of amorphous Si and Ge is an important issue both in the formation of ultra-shallow junctions and in photovoltaics. In the former case the relatively high fluences applied in dopant implantation or the use of pre-amorphization implantation lead to the formation of an amorphous layer. In the first stage of annealing the solid phase epitaxial regrowth (SPER) of the amorphous layer takes place. SPER leads to redistribution of dopants, and they are incorporated into the crystal either substitutionally or within clusters containing self-interstitials or vacancies. In Si the SPER process leaves beyond the original amorphous-crystalline interface the end-of-range damage which contains an excess of self-interstitials. During further annealing, free self-interstitials are emitted from the end-of-range damage and may cause an enhanced diffusion of the dopants. It is highly desirable to understand the processes occurring during SPER on the atomic level. This work presents results of classical molecular dynamics simulations of SPER in pure Si and Ge. While in the last decade several authors investigated SPER in Si, the regrowth of amorphous Ge layers has not been considered yet.
First of all a realistic atomic system with two amorphous-crystalline interfaces which are nearly parallel to a {100} plane is prepared and characterized. The structural properties of the amorphous and crystalline parts are in very good agreement with experimental data from literature. After preparation at 300 K the system is heated to a given temperature and the regrowth of the amorphous layer is monitored by different methods including visualization and statistical analysis. Two stages are found: The initial stage (0 - 3 ns) corresponds to the SPER process. Here, the amorphous part is contiguous and its thickness is large enough so that the two interfaces do not influence each other. In the final stage (4 - 5 ns) the amorphous region becomes thinner, and finally isolated amorphous regions may exist and recrystallize independently of each other. This may lead to the generation of stacking faults and defects. For a wide temperature range regrowth velocities are calculated for the SPER process and the results are drawn in an Arrhenius plot. From this presentation the effective activation energy of SPER and the corresponding pre-exponential factor are determined. The results are compared to experimental data from literature. Furthermore, the evolution of the roughness and the morphology of the amorphous-crystalline interface are investigated.
Keywords: silicon germanium recrystallization atomistic simulation
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Lecture (Conference)
XIIIth International Autumn Meeting on Gettering and Defect Engineering in Semiconductor Technology (GADEST 2009), 26.09.-02.10.2009, Döllnsee-Schorfheide, Germany
Permalink: https://www.hzdr.de/publications/Publ-13257
Intrinsic and extrinsic diffusion of indium in germanium
Kube, R.; Bracht, H.; Chroneos, A.; Posselt, M.; Schmidt, B.
Abstract
Diffusion experiments with indium (In) in germanium (Ge) were performed in the temperature range between 550 and 900 °C. Intrinsic and extrinsic doping levels were achieved by utilizing various implantation doses. Indium concentration profiles were recorded by means of secondary ion mass spectrometry and spreading resistance profiling. The observed concentration independent diffusion profiles are accurately described based on the vacancy mechanism with a singly negatively charged mobile In-vacancy complex. In accord with the experiment, the diffusion model predicts an effective In diffusion coefficient under extrinsic conditions that is a factor of 2 higher than under intrinsic conditions. The temperature dependence of intrinsic In diffusion yields an activation enthalpy of 3.51 eV and confirms earlier results of Dorner et al. [Z. Metallk. 73, 325 (1982)]. The value clearly exceeds the activation enthalpy of Ge self-diffusion and indicates that the attractive interaction between In and a vacancy does not extend to third nearest neighbor sites which confirms recent theoretical calculations. At low temperatures and high doping levels, the In profiles show an extended tail that could reflect an enhanced diffusion at the beginning of the annealing.
Keywords: diffusion indium germanium
- Journal of Applied Physics 106(2009), 063534
Permalink: https://www.hzdr.de/publications/Publ-13256
Tests of ELBE RF-Components with Increased RF-Power
Büttig, H.; Arnold, A.; Büchner, A.; Freitag, M.; Lehnert, U.; Michel, P.; Schurig, R.; Staats, G.; Teichert, J.; Voigtländer, J.; Winter, A.
Abstract
The RF-system of the superconducting electron linac ELBE (40 MeV, 1 mA CW) is in permanent operation since 2001, but it is not completely free of RF-trips. Experience gained within eight years of operation shows that the better the RF-components were conditioned the better is their electrical stability during long time operation. To be prepared for the planned ELBE upgrade with 16 kW of RF-power per cavity several test benches have been built to study the performance of RF-couplers and waveguide windows. In cooperation with Bruker BioSpin / France and CPI / USA the prototype of a 30 kW RF-amplifier based on an IOT had been tested with beam at ELBE. This paper gives an overview about tests of RF-components with increased RF-power at ELBE.
Keywords: ELBE-RF System; Superconducting Radio Frequency; RF 1.3 GHz; RF-Power Coupler; 1.3GHz Waveguide Window; RF-Coupler Test Bench; Resonant Ring (1.3GHz); 1.3GHz CW-RF
Involved research facilities
- SRF Gun
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Poster
14-th International Conference on RF Superconductivity,SRF09 20.-25.09.2009, 20.-25.09.2009, Berlin, Dresden, Deutschland -
Contribution to proceedings
14th International conference on RF Superconductivity, SRF09, 20.-25.09.2009, Berlin, Dresden, Deutschland
Proceedings SRF 2009
Permalink: https://www.hzdr.de/publications/Publ-13255
Side Effects on the Heart and Skeleton of Growing Mice Attributed to Chronic Imatinib Exposure
Suttorp, M.; Boehme, J.; Vaitl, J.; Mosch, B.; Pursche, S.; Jung, R.; Bergmann, R.; Fischer, R.; Pietzsch, J.; Bornhaeuser, M.; Gasser, J. A.
Abstract
Objectives: Chronic myeloid leukemia (CML) is effectively treated by Imatinib (IM) via inhibition of the BCR-ABL tyrosine kinase. However, also related tyrosine kinases like abl, c-Kit, PDGF-R, and c-FMS are blocked by IM. As shown in adult humans and mice, abl-controlled protein folding as part of the endoplasmatic stress response in heart myoblasts as well as bone "remodeling" depending on PDGF-R and c-FMS is impaired under imatinib exposure (Dewar AL et al 2005, Kerkelä R et al 2006, Fitter S et al 2008). The influence of IM on the growing heart and skeleton of immature animals has not been studied so far. With respect to treatment of pediatric CML we report alterations in these organs of juvenile mice chronically exposed to IM during the growth period.
Methods: From the age of 414 weeks (w) [development milestones of mice: weaning 3 w; puberty 7 w; epiphysial lines closure 18 w] C3H/Neu male and female wild-type mice were chronically exposed to IM via the drinking water at concentrations of 500 mg/l (group A), 750 mg/l (group B), and 1000mg/l (group C). Femur length and overall skeletal development was analysed by whole body X-ray analysis using a mammography device. Bone metabolic activity was assessed by total body Na18F PET and CT after 5w and 10w of exposure using dedicated small animal tomographs. Bone mineral density and microstructure of tibiae were analysed by pQCT and microCT (resolution 12.5µ m) while the number of osteoclasts and resorption lacunae in femora and vertebrae was assessed by histomorphometry. Plasma concentration of IM, osteocalcin, and activity of the tartrate resistant acid phosphatase (TRAP5b) was also determined. The heart was examined histologically and ultrastructurally by electron microscopy.
Results: IM was tolerated well and mean uptake of 80 mg/kg/d
A. 110 mg/kg/d
B. and 150 mg/kg/d
C. resulted in serum levels of 60674 ng/ml, 36242 ng/ml and 51534 ng/ml, respectively.
Body weight gain was delayed in groups B and C until the age of 8 w while no change in overall growth, development and behaviour was observed at 14 w. At higher doses of IM and at younger age there was a non-significant trend to a reduction in femur length. Heart morphological examination exhibited an increased number (p<0.05) of hypertrophic cardiomyocytes (toxic damage) paralleled by ultrastructural alterations in mitochondria, myofibrils, and nucleus. In the skeleton, no significant differences compared to controls concerning 18F-kinetics and uptake in vertebrae and femura could be demonstrated. However, IM dose-dependently reduced the number of osteoclasts and resorption lacunae (p<0.05); these effects were less pronounced in female mice. Tibia cortical thickness was increased significantly in males by 6.1% (B) and 11.2% (C), respectively, and 7.5% in females (C). By microCT cancellous bone exhibited a significant increase in trabecular bone mass density and volume and number resulting in an increase in trabecular connectivity in males by 63% (B) and 64% (C), respectively, and in females by 22% (B) and 38% (C), respectively. Bone biomarkers indicated a significant reduction of TRAP5b activity while osteocalcin levels remained unchanged.
Conclusion: In juvenile mice, a chronic exposure of IM resulted in toxic damage of the cardiomyocytes at higher dose rates. However, these alterations do not necessarily imply also a functional impairment which can only be studied in vivo. In the skeleton, IM reduced the number of osteoclasts and resorption lacunae in long bones but not in vertebrae. IM showed an antiresorptive effect in cancellous bone and increased cortical thickness and trabecular number by inhibiting the expansion of the marrow cavity. The effects were more pronounced in male mice and at younger age.
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Poster
Annual Meeting American Society of Hematology, 06.-09.12.2008, San Francisco, USA -
Abstract in refereed journal
BLOOD 112(2008), 402
Permalink: https://www.hzdr.de/publications/Publ-13254
NMR Studies and Crystal Structure Determinations of CF3 Group-containing Bicyclic phenolates
Mamat, C.; Reinke, H.; Langer, P.
Abstract
Three new CF3-substituted bicyclic Salicylate derivatives were synthesized by the TiCl4-mediated cyclization Of trifluoromethyl-containing ketones with 1,3-bis(silyl enol ethers) and characterized by NMR and IR, spectroscopy, Mass spectrometry and elemental analysis. The crystal structures of the bicyclic derivatives have been determined by single crystal X-ray analysis. All structures exhibit hydrogen bonding.
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Zeitschrift für Naturforschung Section B 64(2009)4, 423-426
ISSN: 0932-0776
Permalink: https://www.hzdr.de/publications/Publ-13252
Luminescence properties of uranium(VI) citrate and uranium(VI) oxalate species and their application for the determination of complex formation constants
Günther, A.; Steudtner, R.; Schmeide, K.; Bernhard, G.
Abstract
For the first time, the interaction of uranium(VI) with citric acid and oxalic acid in aqueous solution was investigated using time-resolved laser-induced fluorescence spectroscopy (TRLFS) between pH 2 and 4. The complex species UO2cit− and (UO2)2(cit)22− formed in citrate medium as well as UO2ox and UO2(ox)22- formed in oxalate medium show no luminescence emissions at room temperature. However, by coupling the fluorescence measurement technique with a low temperature system (-120 °C, cryo-TRLFS), emission signals of the various complex species could be detected. The emission signals are bathochromic shifted in comparison to the emission maxima of the uncomplexed uranyl(VI) cation. Using the spectroscopic data, the corresponding complex formation constants were calculated, which corroborate literature data.
Keywords: uranium(VI); citric acid; oxalic acid; time-resolved laser-induced fluorescence spectroscopy; cryogenic measurement technique
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Radiochimica Acta 99(2011), 535-541
DOI: 10.1524/ract.2011.1847
Cited 28 times in Scopus
Permalink: https://www.hzdr.de/publications/Publ-13251
QCD Sum Rules for D and Ds Mesons in Dense and Hot Nuclear Matter
Hilger, T.
Abstract
Tool: QCD sum rules, Goal: D mesons → CBM / FAIR, Outlook: charm near Tc
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Lecture (Conference)
International Conference on Strangeness in Quarkmatter 09 (SQM 09), 27.09.-02.10.2009, Buzios, Brazil
Permalink: https://www.hzdr.de/publications/Publ-13250
Radiokupfer-markierte Peptide auf der Basis neuer bifunktioneller Chelatliganden
Stephan, H.; Bergmann, R.; Steinbach, J.
Abstract
Die erfolgreiche klinische Anwendung von radioaktiv markierten Somatostatin-Peptid-Analogen für die Bildgebung von rezeptorexprimierenden Tumoren hat die Modifizierung anderer Regulatorpeptide wie Neurotensin, RGD-Peptide oder Bombesin als mögliche Tumordiagnostika und therapeutika vorangetrieben.[1] Auf dem Weg zu diesen neuen radioaktiven Arzneimitteln sind eine Reihe unterschiedlicher Aufgaben zu lösen. Das betrifft insbesondere die Entwicklung von chemisch und radiolytisch stabilen Verbindungen, die eine unkomplizierte Markierung der Peptide mit geeigneten Radionukliden erlauben. 99mTc-, 64Cu- und 68Ga-markierte Peptide eignen sich dabei prinzipiell zur Tumordiagnostik. Analoge Verbindungen mit den Partikelstrahlern 67Cu und 188Re weisen ein großes Potenzial zur Therapie von Tumoren auf. Zur stabilen Fixierung von radioaktiven Kupfernukliden sind beispielsweise Pyridin-haltige makrocyclische Amine I und Bispidin-Liganden II entwickelt worden, die gleichzeitig eine Konjugation von Peptiden erlauben. Auf der Basis stabilisierter Bombesinderivate konnten durch Anwendung geeigneter Peptidkupplungsreaktionen entsprechende Biokonjugate hergestellt werden. Diese Verbindungen bilden unter physiologischen Bedingungen mit schneller Kinetik sehr stabile Radiokupferkomplexe. Ligandenaustauschexperimente und radiopharmakologische in-vitro- und in-vivo-Untersuchungen belegen eine sehr hohe Komplexstabilität. Studien zur Bioverteilung eines Bombesinkonjugates mit I ergaben eine hohe Anreicherung im Pankreas, dem Zielorgan mit der höchsten Dichte am Gastrin Releasing Peptidrezeptor.[2] PET-Studien an PC3-Tumor-Mäusen unter Einsatz des 64Cu markierten Bispidin-Bombesin-Derivates belegen eine gute Tumoranreicherung dieser Verbindung sowie eine klare Visualisierung des Tumors.[3]
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Lecture (Conference)
GDCh-Wissenschaftsforum Chemie 2009, 30.08.-02.09.2009, Frankfurt/M., Deutschland
Permalink: https://www.hzdr.de/publications/Publ-13249
Autoradiographic studies of rhenium-188-hydroxyethylidine diphosphonate in normal skeleton and osteoblastic bone metastases in a rat model of metastatic prostate cancer
Liepe, K.; Geidel, H. H.; Bergmann, R.; Haase, M.; Runge, R.; Kotzerke, J.
Abstract
Aim
The quantitative distribution of bone-seeking radiopharmaceuticals in trabecular bone, cortical bone and in skeletal metastases is required for calculation of radiation-absorbed dose in radionuclide therapy. An animal model of intraosseous tumor cell administration was developed to simulate osteoblastic metastases for autoradiographic study of radionuclide localization.
Methods In 45 Copenhagen rats R3327-MATLyLu syngeneic prostate cancer cells were given intraosseously in both the femori. Rhenium-188-hydroxyethylidine diphosphonate (HEDP) was administered intravenously 17 +/- 1 days after cells instillation and these animals were euthanized at 4, 24 and 48 h after injection of the radiopharmaceutical. The uptake of radiopharmaceutical was estimated in normal skeleton and the bone metastases by means of region of interest analysis using autoradiography. The tumor to nontumor ratio and the fractional uptake in cortical bone and trabecular bone were quantified.
Results
The uptake of rhenium-188-HEDP in cortical bone was 33.5% and in trabecular bones was 66.5% after 4 h, 34.6 and 65.4% after 24 h, and 35.9 and 64.1% after 48 h, respectively. Assuming a theoretic cortical-trabecular distribution of 50-50%, (MIRDOSE) calculation, radiation-absorbed dose to bone marrow was underestimated by 26%. In bone metastases, an inhomogeneous distribution with a minimal and maximal tumor to nontumor ratio of 3:1 and 14:1 after 4 h, 5: 1 and 14: 1 after 24 h, and 5:1 and 16:1 after 48 h was observed.
Conclusion
The MIRDOSE model underestimates the radiation-absorbed dose to the bone marrow because of demonstrable differences in the uptake of rhenium-188-HEDP in cortical and trabecular bone and inhomogeneous uptake in skeletal metastases.
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Nuclear Medicine Communications 30(2009), 693-699
DOI: 10.1097/MNM.0b013e32832cc23c
ISSN: 0143-3636
Cited 9 times in Scopus
Permalink: https://www.hzdr.de/publications/Publ-13248
Prätherapeutisches [18F]FMISO hypoxisches Volumen ist ein signifikanter prognostischer Faktor für die lokale Tumorkontrolle nach Einzeldosisbestrahlung von FaDu-Tumoren in Nacktmäusen/Pretherapeutic [F-18]FMISO hypoxic volume is a significant prognostic factor for local tumour control after single dose radiation of FaDu- tumours in night mouse
Schütze, C.; Bergmann, R.; Mosch, B.; Yaromina, A.; Zips, D.; Hessel, F.; Thames, H. D.; Mäding, P.; Kotzerke, J.; Baumann, M.; Beuthien-Baumann, B.
Abstract
Hintergrund:
Präklinische und klinische Untersuchungen haben gezeigt, dass das Ausmaß der prätherapeutischen Tumorhypoxie das Ergebnis einer Strahlentherapie solider Tumoren beeinflusst. Derzeit werden strahlentherapeutische Interventionen wie z. B. Dosis-Eskalation partieller hypoxischer Subvolumina untersucht. In dieser Studie wurde in einer einzelnen, in Nacktmäusen transplantierten humanen Tumorzelllinie untersucht, ob das prätherapeutische [18F]FMISO hypoxische Tumorvolumen (HV) oder die Intensität des Tracer-uptakes (maximaler Standard uptake
value SUVmax) mit der lokalen Tumorkontrolle nach Einzeldosisbestrahlung korreliert.
Methoden:
Die hSCC Zelllinie FaDu wurde subkutan auf das rechte Hinterbein von NMRI Nacktmäusen transplantiert. 70 Tiere wurden bei einem Tumorvolumen von 165-343 mm³ in das Experiment aufgenommen. Jedes Tier erhielt am Tag 0 eine PET-Untersuchung (MicroPET® P4, CTI Molecular Imaging Inc) mit dem Hypoxie-Marker 18F]FMISO ([18F]Fluormisonidazol) unter Anästhesie. Die Auswertung erfolgte mittels 3D-regions of interest über dem Tumor (ROVER software, ABX GmbH, Radeberg, Germany). Bestimmt wurde das [18F]FMISO hypoxische Volumen (HV) und der SUVmax. Anschließend wurden die Tumoren entsprechend des medianen hypoxischen Volumens für Einzeldosisbestrahlungen mit 25 Gy oder 35 Gy unter normalem Blutfluss randomisiert. Die Einzeldosisbestrahlungen erfolgten mit 200 kV Röntgenstrahlen (0.5 mm Cu, ~ 1 Gy min-1). Der experimentelle Endpunkt war die lokale Tumorkontrolle am Tag 120 nach Bestrahlung.
Ergebnisse:
Die lokalen Tumorkontrollraten nach Bestrahlung mit 25 Gy waren niedriger als nach Bestrahlung mit 35 Gy (22% vs. 69%, Logrank-Test p< 0.0001). Die Spanne der HV reichte von 38-353 mm³, der Median HV betrug 112 mm³ (95%CI: 92; 128 mm³). Für Tumoren < Median HV betrug die lokale Kontrollrate 33% nach 25 Gy vs. 82% nach 35 Gy (p=0.001). In Tumoren > Median HV betrug die lokale Kontrollrate 15% nach 25 Gy vs. 53% nach 35 Gy (p=0.0005). In der multivariaten Cox-Analyse konnte nach Korrektur für Dosis und Tumorvolumeneffekte ein signifikanter Effekt des HV als kontinuierliche Variable (p=0.009) oder dichotome Variable (Stratifikation entsprechend des Median HV) (p=0.039) nachgewiesen werden. Der SUVmax war bezüglich der Prognose der Heilungswahrscheinlichkeit nicht relevant.
Schlussfolgerungen:
Das [18F]FMISO hypoxische Tumorvolumen ist ein signifikanter unabhängiger Prädiktor für das Ergebnis einer Bestrahlung mit hohen Einzeldosen in FaDu hSCC. Diese Ergebnisse unterstützen die Hypothese, dass ein prätherapeutisches [18F]FMISO-PET wichtige Informationen für die Verschreibung einer heterogenen Bestrahlungsdosis in
hypoxischen Subvolumina individueller Tumoren liefern kann. Weitere Experimente mit anderen Tumormodellen und fraktionierter Bestrahlung sind notwendig.
Gefördert im Rahmen des EU-Projektes BioCare Molecular Imaging for Biologically Optimized Cancer Therapy proposal# 505785 und DFG Projekt Ba 1433.
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Lecture (Conference)
DEGRO 2009 - 15. Jahreskongress der Deutschen Gesellschaft für Radioonkologie, 11.-14.06.2009, Bremen, Deutschland -
Abstract in refereed journal
Strahlentherapie und Onkologie 185(2009)Suppl. 1, 22-23
ISSN: 0179-7158
Permalink: https://www.hzdr.de/publications/Publ-13247
InIII and GaIII Complexes of Sugar-Substituted Tripodal Trisalicylidene Imines: The First 68Ga-Labelled Sugar Derivative
Gottschaldt, M.; Bohlender, C.; Pospiech, A.; Görls, H.; Walther, M.; Müller, D.; Klette, I.; Baum, R. P.; Schubert, U. S.
Abstract
Gallium and indium complexes derived from salicylaldimines of 1,1,1-tris(aminomethyl)ethane (TAME) with pendantxylose, glucose and galactose units have been synthesised as model compounds for potential application as radiotracers. The formed neutral complexes have been characterised by NMR spectroscopy, elemental analysis, mass spectrometry and, in the case of the galactose-bearing InIII complex, by single-crystal X-ray structure analysis. Octahedral coordination was observed with the appearance of an equilibrium of - and -isomers at the metal centre. The glucose-appended ligand was radiolabelled with 68GaIII ions in up to 98 % yield depending on the prevailing pH value. The in vitro stability of the radioactive complex was examined by challenge experiments against apo-transferrin and blood plasma. Very high stability was observed; even after a period of 2 h, 90 % of the complex could still be detected.
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European Journal of Inorganic Chemistry 28(2009), 4298-4307
DOI: 10.1002/ejic.200900561
Cited 7 times in Scopus
Permalink: https://www.hzdr.de/publications/Publ-13246
Circulating S100A12: a novel player in atherosclerosis?
Pietzsch, J.
Abstract
S100A12 is a member of the S100 family of EF-hand calcium-binding proteins. Besides calcium binding S100A12 also shows high affinity for zinc and copper ions. Extracellular S100A12 is predominantly secreted by granulocytes and monocytes and is part of the innate immune response.
S100A12 is markedly overexpressed in inflammatory compartments, and elevated serum levels of S100A12 are found in patients suffering from various inflammatory and metabolic disorders. In this regard, binding of copper by S100A12 is assumed to play a pathogenic role. In vitro experiments show that copper-bound S100A12 can function as a pro-oxidant agent by supporting both copper reduction and copper redox-cycling, respectively. As a consequence, copper-bound S100A12 enhances and accelerates oxidation of human low density lipoprotein lipids and apolipoproteins, respectively. Furthermore, copper-bound S100A12 stimulates proinflammatory activation of endothelial cells, granulocytes, and monocytes. These processes were substantially suppressed in the presence of redox-inert copper-chelating or radical-scavenging agents. Clinical examinations show significantly elevated plasma S100A12 levels in subjects with impaired glucose tolerance, newly-diagnosed diabetes mellitus Type 2, and acute rheumatoid arthritis (1.5 to 3-fold higher than in control subjects). In the patient groups, plasma S100A12 is strongly associated with plasma markers of both LDL oxidation and inflammation, and, additionally, with ultrasonically measured carotid atherosclerosis. It is suggested that oxidation processes mediated by copper-bound S100A12 are involved in accelerated atherogenesis in proinflammatory states.
Supported by Deutsche Forschungsgemeinschaft (Pi 304/1-1)
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Invited lecture (Conferences)
11th International Congress on Amino Acids, Peptides and Proteins, 03.-07.08.2009, Wien, Österreich -
Abstract in refereed journal
Amino Acids 37(2009)Suppl. 1, S78
DOI: 10.1007/s00726-009-0320-1
ISSN: 0939-4451
Permalink: https://www.hzdr.de/publications/Publ-13245
Molecular imaging of the receptor for advanced glycation endproducts
Pietzsch, J.; Hoppmann, S.
Abstract
The receptor for advanced glycation endproducts (RAGE) is a member of the immunoglobulin superfamily and has been implicated in the pathogenesis of various disorders including inflammatory processes and cancerogenesis. However, data concerning the functional expression of RAGE in inflammatory compartments and other pathologies in vivo are scarce. We report a multi-radiotracer approach using radiolabeling of various RAGE ligands, including glycated low-density lipoproteins (glycLDL), glycated albumin (glycBSA), and S100 proteins (S100B and S100A12) with the positron emitter fluorine-18 (18F) and the application of 18F-labeled RAGE ligands in dynamic small animal positron emission tomography (PET) studies. Radiolabeling of proteins was performed by conjugation with N-succinimidyl-4-[18F]fluorobenzoate ([18F]SFB) causing no adverse alterations of the biological functionality of the proteins in vitro. Biodistribution and metabolite studies in rodent normal, inflammatory, and tumor models revealed high stability for the 18F-RAGE ligands in vivo. The in vivo kinetics of 18F-RAGE ligands, with or without presence of specific ligands or inhibitors of RAGE and, additionally, various scavenger receptors, in rodent models was quantified by PET, and correlated well with the anatomical localization of RAGE, e.g., in lung, endothelium, inflammatory lesions, and tumors.
18F-radiolabeling of glycLDL, glycBSA, and S100 proteins and the use of small animal PET provide a potential approach to measure the functional expression of RAGE under normal and pathophysiological conditions in vivo.
Supported by Deutsche Forschungsgemeinschaft (Pi 304/1-1)
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Invited lecture (Conferences)
11th International Congress on Amino Acids, Peptides and Proteins, 03.-07.08.2009, Wien, Österreich -
Abstract in refereed journal
Amino Acids 37(2009)Suppl. 1, S39
DOI: 10.1007/s00726-009-0320-1
ISSN: 0939-4451
Permalink: https://www.hzdr.de/publications/Publ-13244
Fluorine-18 radiolabeling of S100/calgranulins: potential probes for molecular imaging of receptor for advanced glycation endproducts
Hoppmann, S.; Haase, C.; Richter, S.; Strobel, K.; Steinbach, J.; Pietzsch, J.
Abstract
The interaction of S100/calgranulins, a multigenic family of Ca2+-modulated proteins, with the receptor for advanced glycation endproducts (RAGE) is hypothesized to be of high relevance in the pathogenesis of various diseases including cardiovascular diseases, inflammatory processes, and cancerogenesis. However, data concerning the role of circulating S100 proteins in these pathologies are scarce. Furthermore, it is currently not known whether RAGE is an universal S100 receptor. One reason for this is the shortage of suitable radiolabeling methods for direct assessment of the metabolic fate of circulating S100 proteins in vivo. We report a novel radiotracer approach using radiolabeling of recombinant human S100A1 with the positron emitter-fluorine-18 (18F) by conjugation with N-succinimidyl-4-[18F]fluorobenzoate ([18F]SFB) and the use of [18F]fluorobenzoylated S100A1 (18F-S100A1) in dynamic small animal positron emission tomography (PET) studies in rats. Human S100A1 was cloned as a fusion protein in the bacterial expression vector pGEX-6P-1 and expressed in E. coli strain BL21. Radiolabeling of S100A1 with [18F]SFB at pH 7.4 resulted in 18F-S100A1 specifically labeled at the N-terminal glycine residue with radiochemical yields of 2-6% (decay-corrected) and effective specific activities of 0.5-1 GBq/µmol, respectively. In vitro experiments, and biodistribution and metabolite studies in rats in vivo revealed high stability for the 18F-S100A1. The metabolic fate of 18F-S100A1 in rats in vivo was delineated by dynamic PET studies using a dedicated small animal PET system. The organ-specific in vivo distribution and kinetics of 18F-S100A1 correlated well with the anatomical localization of RAGE, e.g., in lungs and in the vascular system. In the presence of molar excess of glycated human low density lipoprotein (glycLDL), a well characterized RAGE ligand, the mean plasma residence time of circulating 18F-S100A1 increased by 40% from 29.6 ± 1.5 min to 41.3 ± 2.1 min and, vice versa, tissue-associated retention of 18F-S100A1 decreased by approximately 50% in lungs and 32% in large blood vessels, respectively. These findings indicate first circulating S100A1 to be a specific ligand for RAGE in rats in vivo. In conclusion, radiolabeling of S100/calgranulins with 18F and the use of small animal PET provide novel probes to delineate functional expression of RAGE under normal and pathophysiological conditions in rodent models of disease in vivo.
Keywords: multiligand receptors; pattern recognition; S100 proteins; 18F-labeled prosthetic group; small animal positron emission tomography; animal models
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Contribution to external collection
Xiaoyuan Chen: Recent Advances of Bioconjugation Chemistry in Molecular Imaging, Kerala (India): Trivandrum: Research Signpost, 2008, 978-81-308-0210-7, 329-351
Permalink: https://www.hzdr.de/publications/Publ-13243
Synthesis, 64Cu-Labeling and Biodistribution of DOTA-Glycodendrimers
Jäger, K.; Stephan, H.; Bergmann, R.; Steinbach, J.; Appelhans, J.; Voit, D.
Abstract
The utilization of dendrimers in medicine holds great potential in emerging applications of diagnostic imaging, as well as the promise of new capabilities for delivering therapies tailored and targeted for specific diseases. In this perspective, radiolabeled dendritic frameworks are gaining in importance, particularly for the use in tumor imaging and therapy.[1] Pegylation as well as carbohydration of radiolabeled compounds is of considerable interest to improve the pharmacokinetics, biocompatibility, and tumor accumulation.[2,3]
In this context, DOTA-modified glycodendrimers with dense maltose shell (Figure: structure of 4th generation dendrimer) were selected from the point of view to use the highly homogenous dendritic structure for improved tumor imaging and therapy and to enhance the biocompatibility of dendrimers by the decoration with carbohydrates. The outcome of the synthetic effort was the synthesis of 4th and 5th generation glycodendrimers with the variation of chemically attached DOTA chelators (1, 3, 9 DOTA units/4th generation dendrimer; 9 and 18 DOTA units/5th generation dendrimer), which form stable complexes with a large number of radiometals. The multivalent decoration with DOTA on dendrimer surface was also stimulated by the facts that radiolabeling kinetics can be accelerated and to achieve enhanced specific activity.
The labeling conditions of the glycodendrimers synthesized with 64Cu were optimized, and the influence of reaction time, temperature, buffer conditions and the dendrimer amount on the radiochemical yield were studied using Radio-TLC and Radio-SEC. The radiocopper(II) complexes of the DOTA-functionalized glycodendrimers show a high in vitro stability. Preliminary biodistribution studies of 64Cu-labeled 4th generation dendrimers with maltose shell in healthy Wistar rats indicate the preferred accumulation in the liver.
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Poster
GDCh-Wissenschaftsforum Chemie 2009, 30.08.-02.09.2009, Frankfurt am Main, Deutschland
Permalink: https://www.hzdr.de/publications/Publ-13242
Visualizing inflammation activity in rheumatoid arthritis with Tc-99m Anti-CD4-mAb fragment scintigraphy - First results of a proof of principle study
Steinhoff, K.-G.; Pierer, M.; Sorger, D.; Seese, A.; Künstler, J. U.; Emmrich, F.; Sabri, O.; Hesse, W.; Siegert, J.; Piegla, U.; Pietzsch, H.-J.; Seidel, W.; Laub, R.
Abstract
T‐cell‐located CD4 antigen represents one of the therapeutic targets in rheumatoid arthritis (RA). However, up to now it has not been possible to visualize this target in vivo. The aim of our study was to assess the safety and tolerability of a Technetium 99 labelled anti‐CD4 antibody fragment (Tc‐99m‐anti‐CD4) in patients with active synovitis due to rheumatoid arthritis and to evaluate its potential as a marker of disease activity. Methods: In the present phase I proof of principle study 5 patients (3 female, 2 male, 58 to 71 years) with RA were examined. Planar whole body scans as well as separate hand and feet scintigraphies were taken 30 minutes, 1, 2, 4, 8 and 24 hours after application of 585 +/‐ 115 MBq Tc‐99m‐anti‐CD4. The obtained scintigramms were analysed visually and compared with clinical data in 68 joints per patient. Active inflammation was clinically defined by swelling and tenderness in at least one joint (gold standard). Patients were clinically re‐evaluated 7 days p.i. Results: Neither infusion related adverse events nor adverse events during follow up were observed. No increase in HAMA titres was seen. All 5 patients had positive scans in 25 of 37 clinically affected joints. Positive scans were also found in 19 out of 227 joints without evidence of swelling or tenderness yielding a 7% rate of false positive joints and a 32% rate of false negative joints. Conclusion: Scintigraphy with Tc‐99m‐anti‐CD4 is a new promising technique for evaluation of inflammatory activity in patients with RA. Tracer uptake in clinically inconspicuous joints strongly indicates diagnostic potential of 99Tc anti CD4. Based on the few patients investigated, it seems that inflammation is detected with apparently higher specificity than sensitivity. Whether this technique is eligible for prognostic disease evaluation needs to be analysed in further studies as well as the pathophysiological background of clinically affected joints lacking tracer uptake.
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Lecture (Conference)
Annual Congress of the European Association of Nuclear Medicine 2009 (EANM), 10.-14.10.2009, Barcelona, Spain -
Abstract in refereed journal
European Journal of Nuclear Medicine and Molecular Imaging 36(2009)Suppl. 2, S210
ISSN: 1619-7070
Permalink: https://www.hzdr.de/publications/Publ-13241
Synthesis and biological evaluation of new [Tc(N)(R2PS)]-based mixed compounds as analogues of WAY 100635
Bolzati, C.; Cavazza-Ceccato, M.; Refosco, F.; Salvarese, N.; Pietzsch, H.-J.; Bergmann, R.; Bandoli, G.
Abstract
Aim: This study was focused on evaluating the applicability of a new labelling procedure to the preparation of Tc(N)‐based target specific compounds. The chemistry is based on the use of the [Tc(N)Cl(R2PS)(PPh3)] species (R2PS = alkyl‐phosphino‐thiolate ligand), which selectively reacts with an appropriate mono‐negative chelate, such as a dithiocarbamate (DTC), to give neutral [Tc(N)(R2PS)(DTC)] compounds. The 2‐methoxyphenylpiperazine (2‐MPP) pharmacophore, which displays a potent and specific affinity for 5HT1A receptors, was selected as functional group and conjugated to the dithiocarbamate unit through different spacers. Method: The synthesis of [99m/99gTc(N)(R2PS)(Ln)] complexes, and their in vitro stability as well as their biological in‐vitro and in‐vivo assays were investigated. Stability studies were performed by considering: i) stability toward transchelation with Cysteine and Glutatione ii) binding to the serum proteins; ii) stability in rat serum, human serum and rat liver homogenates. The in vitro affinity for the 5HT1A receptors of the technetium complexes was assessed by measuring the ability of the compounds to compete with [3H]‐8‐OH‐DPAT binding in isolated membranes from rat cerebral cortex. The biodistribution profile of the best radiolabeled compound and its in vivo stability were evaluated in Sprague‐Dawley rats. Results: [99mTc(N)(R2PS)(Ln)] complexes were prepared in high yield (>90%) using a multi‐step procedure. The chemical identity of 99mTc‐complexes was determined by HPLC comparison with the corresponding 99gTc‐complexes. All complexes were found to be inert toward transchelation with an excess of free Glutathione and Cysteine. No significant in vitro serum protein binding and no notable biotransformation of the native compound into different species by the in vitro action of the serum and liver enzymes were shown. Nanomolar affinities for the 5‐HT1A receptor were obtained for [99mTc(N)(PSiso)L3] (IC50 = 1.5 nM), a reduction of the affinity were observed for the other complexes as a function of the reduction of the alkyl chain length interposed between the DTC group and the bioactive molecule. A negligible brain uptake was displayed from in vivo distribution data of [99mTc(N)(PSiso)L3]. Conclusion This work describes the application of a new labelling procedure for incorporating a bioactive molecule into a stable dissymmetric 99mTc(N)‐complex. Despite the favourable binding properties, the lack of BBB penetration indicates that these particular complexes may not be useful for CNS‐receptor mapping. Further studies should be performed in order to clarify the reason for this behaviour and to evaluate the usefulness in peripheral applications.
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Lecture (Conference)
Annual Congress of the European Association of Nuclear Medicine (EANM) 2009, 10.-14.10.2009, Barcelona, Spain -
Abstract in refereed journal
European Journal of Nuclear Medicine and Molecular Imaging 36(2009)Suppl. 2, S220
ISSN: 1619-7070
Permalink: https://www.hzdr.de/publications/Publ-13240
Photochemistry of uranium(VI) revisited: A density functional theory study
Tsushima, S.; Fahmy, K.
Abstract
Photochemical reduction of uranium(VI) in the presence of organic substances is a well known and well studied process, but its reaction mechanism has not yet been fully verified. One of the difficulties in studying uranium photochemistry is the involvement of photo-excited states which is difficult to assess solely by experiments. Quantum chemical calculation is capable of predicting the properties of excited state uranium(VI), and therefore can provide possible photochemical reaction mechanisms and reaction pathways. Here, we have studied the photochemical reduction of uranium(VI) in the presence of several organic ligands, namely methanol, ethanol, and oxalic acid, by density functional theory (DFT) calculations. We were able to reproduce entire reaction pathways which demonstrates the validity of the DFT approach in further exploring uranium(VI) photochemistry.
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Lecture (Conference)
Spring 2010 National Meeting and Exposition, Symposium on "Lanthanides and Actinides: a Chemist's Perspective", 21.-25.03.2010, San Francisco, U.S.A.
Permalink: https://www.hzdr.de/publications/Publ-13239
Aptamer modifizierte bakterielle Oberflächenstrukturen für die Entwicklung neuer Sensoren (AptaSens)
Pollmann, K.
Abstract
Bakterielle Hüllproteine (S-Layer) werden als Grundlage für die Entwicklung von Biosensoren für die Detektion von Spurenstoffen in Wässern genutzt. Im April startete dazu ein BMBF-Verbundprojekt im Rahmen der Fördermaßnahme Biona. Dieses Projekt wird vorgestellt.
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Lecture (others)
Vortragsreihe GMBU, Arbeitsgruppenberatung, 11.11.2009, Dresden, Deutschland
Permalink: https://www.hzdr.de/publications/Publ-13238
Bispidine als Radiokupferchelatoren - Konfigurationsisomerie Imidazol-haltiger Derivate
Fähnemann, S.; Juran, S.; Matterna, M.; Walther, M.; Stephan, H.; Emmerling, F.; Kraus, W.
Abstract
Derivate des 3,7-Diazabicyclo[3.3.1]nonans (Bispidin) bilden insbesondere mit Cu2+ sehr stabile Koordinationsverbindungen, wobei die Komplexstabilität im Bereich jener mit makrocyclischen Liganden liegt.[1] Für Bispidin-Derivate ergeben sich drei unterschiedliche Konformationsisomere, wobei die abgeflachte Doppel-Sessel-Form die thermodynamisch stabilste Konformation repräsentiert. Dabei sind die beiden Aminstickstoff-Donoratome (N3- und N7-Position) des Bispidin-Grundgerüstes für die Koordination mit Metallionen optimal vororganisiert.
Die Einführung von weiteren Donoreinheiten, wie Pyridyl- oder Imidazolyl-Substituenten, an den Positionen C2 und C4 kann zu Konfigurations-isomeren mit cis- und trans-Stellung führen. Hexadentate Bispidin-Liganden mit vier Pyridin-Einheiten lassen sich mit hoher Ausbeute in der für die Komplexbildung mit Cu2+ gewünschten cis-Isomerie (endo/endo) darstellen. Die entsprechenden 64Cu-Komplexe zeigen sehr interessante radiopharmakologische Eigenschaften.[2] Aufgrund der Komplexbildungs- und Löslichkeitseigenschaften erscheinen in diesem Zusammenhang auch Radiokupfer-komplexe von Imidazol-haltigen Bispidin-Derivaten aussichtsreich.
Es wird darüber berichtet, wie sich die Einführung von Imidazolyl-Substituenten auf die Konfigurationsisomerie von Bispidin-Derivaten auswirkt. Dazu werden insbesondere NMR-spektroskopische Daten und Röntgenkristallstrukturen herangezogen.
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Poster
GDCh-Wissenschaftsforum Chemie 2009, 30.08.-02.09.2009, Frankfurt am Main, Deutschland
Permalink: https://www.hzdr.de/publications/Publ-13237
Imaging and functional characterization of the receptor for advanced glycation endproducts (RAGE) in vivo
Pietzsch, J.; Hoppmann, S.; Richter, S.; Strobel, K.; Steinbach, J.
Abstract
RAGE has been implicated in the pathogenesis of various disorders including inflammatory processes and cancerogenesis. However, data concerning the functional expression of RAGE in inflammatory lesions and other pathologies in vivo are scarce. We report a novel radiotracer approach using radiolabeling of various RAGE ligands, including S100 proteins (S100B/S100A12), glycated low-density lipoproteins (glycLDL), and glycated albumin (glycBSA) with the positron emitter fluorine-18
(18F) and the application of 18F-labeled RAGE ligands in dynamic small animal positron emission tomography (PET) studies. Radiolabeling of proteins was performed by conjugation with no-carrier added N-succinimidyl-4-[18F]fluorobenzoate ([18F]SFB) causing no adverse alterations of the biological functionality of the proteins in vitro.
Biodistribution and metabolite studies in rodent normal, inflammatory, and tumor models revealed high in vivo-stability for the 18F-RAGE ligands. The in vivo-kinetics of 18F-RAGE ligands, with or without presence of specific ligands/inhibitors of RAGE and various scavenger receptors, in rodent models was quantified by PET, and correlated well with the anatomical localization of RAGE, e.g., in blood vessels, lungs, inflammatory lesions, and tumors. 18F-radiolabeling of S100 proteins, glycLDL and glycBSA and the use of small animal PET provide potential probes to measure functional expression of RAGE under normal and pathophysiological conditions in vivo.
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Poster
XXXVI International Congress of Physiological Sciences, 27.07.-01.08.2009, Kyoto, Japan -
Abstract in refereed journal
Journal of Physiological Sciences 59(2009)Suppl. 1, 325
Permalink: https://www.hzdr.de/publications/Publ-13236
The inhomogeneous MUSIG model for upward polydisperse flows with new constitutive models for bubble coalescence and breakup
Liao, Y.; Lucas, D.
Abstract
In the present study we propose new coalescence and breakup closures for the inhomogeneous multiple bubble size group (MUSIG) model. The major purpose is to consider bubble coalescence and breakup due to different mechanisms and to develop a general applicable constitutive model for CFD applications. For bubble coalescence the new model includes coalescence due to turbulence, laminar shear, wake entrainment and eddy capture. Bubble breakup mechanisms encompass turbulent fluctuation, laminar shear and interfacial slip velocity. The new models were implemented in ANSYS-CFX and applied to the case of turbulent air-water mixtures in a large vertical pipe (DN 200). Simulation results for the evolution of radial gas volume fraction, bubble size distribution were compared to as default used closure models of Luo & Svendsen and Prince & Blanch [1, 2] as well as TOPFLOW experimental data. Better prediction of bubble size distribution is accomplished.
Keywords: Inhomogeneous MUSIG model; New constitutive models; Bubble coalescence and breakup; TOPFLOW test facility
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Contribution to proceedings
International Conference Nuclear Energy for New Europe 2009, 14.-17.09.2009, Bled, Slovenia -
Poster
International Conference Nuclear Energy for New Europe 2009, 14.-17.09.2009, Bled, Slovenia
Permalink: https://www.hzdr.de/publications/Publ-13235
Development and validation of bubble coalescence and breakup models : status of KEK project
Liao, Y.; Lucas, D.
Abstract
Bubble coalescence and breakup is an important phenomenon in gas-liquid mixtures. The application of existing models is limited and they are usually not transferable from one case to another. The objective of the work is to develop a generally applicable new model for bubble coalescence and breakup. Based on an extensive literature study, a basis model is proposed which encompasses all important mechanisms. The model is implemented into the Test Solver and CFX code and applied to a case of air-water flow in a vertical pipe. The comparison with the experimental data from TOPFLOW facility shows substantial difference between the results given by Test Solver and CFX. Test Solver with the new model can provide a much better agreement than CFX. This might be caused by the turbulence modeling. The influence of two-phase turbulence parameters will be investigated in future work.
Keywords: Test Solver; Inhomogeneous MUSIG model; New model; Bubble coalescence and breakup; TOPFLOW test facility
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Lecture (Conference)
German CFD Network 16th Meeting, 07.-08.10.2009, Garching, Germany
Permalink: https://www.hzdr.de/publications/Publ-13234
Further developments of the thermodynamic reference database THEREDA and the thermodynamic sorption database RES3T
Richter, A.; Altmaier, M.; Brendler, V.; Marquardt, C.; Moog, H.; Scharge, T.; Voigt, W.; Wilhelm, S.; Wollmann, G.
Abstract
The THEREDA project aims at a consistent and quality assured thermodynamic reference database for modeling geochemical processes in waste disposal sites. It offers evaluated thermodynamic data for all relevant elements, covering both radioactive waste and chemo-toxic substances, and with full bibliographic tracking. Parameters for a variety of models describing interactions in mixed phases are included, too. All host rocks currently discussed as candidates for waste repositories in Germany are considered. THEREDA is freely accessible (www.thereda.de).
The RES³T database (Rossendorf Expert System for Surface and Sorption Thermodynamics) supplies complementary information based on the concept of surface complexation models (SCM). Recently, a portal (www.fzd.de/RES3T) started to provide open public access.
Next steps are the integration of SCM data from RES³T into the THEREDA framework, the provision of data export tools (with speciation-code specific formatting), and the development of a web-based data input and editing interface.
Keywords: THEREDA; RES3T; thermodynamic database; sorption; radioactive waste; chemo-toxic substances; modelling
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Lecture (Conference)
239th ACS National Meeting, 21.-25.03.2010, San Francisco, USA -
Abstract in refereed journal
American Chemical society: Abstracts of scientific papers 239(2010), GEOC-112
ISSN: 0065-7727
Permalink: https://www.hzdr.de/publications/Publ-13230
A Three-Scale Expansion Solution for a Time-Dependent P1 Neutron Transport Problem with External Source
Merk, B.; Weiß, F. P.
Abstract
This work presents the development of an analytical approximation solution for a space-timedependent neutron transport problem in a one-dimensional system consisting of a homogenized medium with a central external source with Greens functions. The delayed neutron production is implemented in two additional timescales with the multiple-scale expansion method. Qualitative results for a given system are analyzed, and a detailed comparison of the developed analytical approximation solution with results gained by the point-kinetics equation and the time-dependent diffusion equation without separation of space and time is given.
Keywords: Time Dependent Neutron Transport; Multiple Scale Expansion; Green's Functions; Accelerator Driven Systems
- Nuclear Science and Engineering 163(2009), 152-174
Permalink: https://www.hzdr.de/publications/Publ-13229
Influence of humic acid functionalities on uranium complexation and influence of humic acid on uranium(VI) migration in opalinus clay
Schmeide, K.; Sachs, S.; Joseph, C.; Raditzky, B.; Bernhard, G.
Abstract
Results are reported to the influence of different humic acid functionalities (nitrogen, sulfur and phosphorus containing functionalities) on the uranium(VI) complexation, to the uranium(IV) complexation by small organic model ligands, to the sorption of uranium(VI) onto opalinus clay in the absence and presence of humic acid and to the uranium(VI) diffusion in opalinus clay in the absence and presence of humic acid.
Keywords: Uranium; humic substances; complexation; functional groups; sorption; opalinus clay
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Lecture (others)
Workshop zum Forschungsvorhaben "Wechselwirkung und Transport von Actiniden im natürlichen Tongestein unter Berücksichtigung von Huminstoffen und Tonorganika", 06.-07.10.2009, Mainz, Germany
Permalink: https://www.hzdr.de/publications/Publ-13228
Anomalous Hall resistance in Ge:Mn systems with low Mn concentrations
Zhou, S.; Bürger, D.; Helm, M.; Schmidt, H.
Abstract
Taking Mn doped Germanium as an example, we evoke the consideration of a two-band-like conduction in diluted ferromagnetic semiconductor (FMS). The main argument for claiming Ge:Mn as a FMS is the occurrence of the anomalous Hall effect (AHE). Usually, the reported AHE (1) is observable at temperatures above 10 K, (2) exhibits no hysteresis, and (3) changes the sign of slope. We observed a similar Hall resistance in Mn implanted Ge with the Mn concentration as low as 0.004%. We show that the puzzling AHE features can be explained by considering a two-band-like conduction in Ge:Mn.
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Applied Physics Letters 95(2009), 172103
DOI: 10.1063/1.3257363
Cited 15 times in Scopus
Permalink: https://www.hzdr.de/publications/Publ-13227
Quantitative myocardial perfusion PET combined with coronary anatomy derived from CT angiography: Validation of a new fusion and visualisation software
Fricke, H.; Elsner, A.; Weise, R.; Bolte, M.; van den Hoff, J.; Burchert, W.; Domik, G.; Fricke, E.
Abstract
Aim
Dynamic perfusion PET offers a clinical relevant advantage over myocardial perfusion scintigraphy due to its ability to measure myocardial blood flow quantitatively. This leads to an improved detection of multivessel disease and the possibility to assess not only the culprit lesion but lower grade stenoses as well. For appropriate revascularization, perfusion defects must be matched to coronary lesions. It has been shown that image fusion of morphological and functional images is superior to side-by-side analysis. Still, software for quantitative perfusion PET combined with CT angiography is rare. In this paper we present a new software tool for image fusion and visualization of quantitative perfusion PET and coronary morphology derived from CT angiography.
Methods
In our software, a PET uptake image is used for manual co-registration. Co-registration results are then applied to the functional data derived from compartment modelling. To evaluate the reproducibility of the manual co-registration, we calculated the deviation between a series of manual co-registrations performed on nine pairs of unregistered PET and CT datasets by five trained participants. Two dimensional transfer functions were used to highlight the coronary arteries from the CT study in the combined data sets.
Results
The average Euclidian distances for three references points were between 3.7 and 4.1 mm. The maximum distance was 10.6 mm. By the use of the two dimensional transfer functions, coronary anatomy could be easily visualised either by user-interaction or automatically by use of neuronal networks.
Conclusions
With this approach it is possible to combine quantitative perfusion PET with coronary anatomy derived from CT angiography. Our first experiences indicate that manual image fusion with our tool is reproducible and that visualisation of the combined datasets is achieved within short time.
Ziel
Die dynamische Perfusions-PET bietet gegenüber der Myokardszintigraphie den klinisch relevanten Vorteil einer quantitativen Perfusionsmessung. Dies führt zu einer besseren Erkennung von Mehrgefäßerkrankungen sowie dazu, dass nicht nur die führenden, sondern auch niedriggradigere Stenosen bezüglich ihrer Relevanz beurteilt werden können. Revaskularisierende Maßnahmen erfordern die korrekte Zuordnung von Perfusionsdefekt und verursachendem Gefäß. Es konnte gezeigt werden, dass die Bildfusion von morphologischer und funktioneller Information einer getrennten Beurteilung überlegen ist. In dieser Arbeit stellen wir eine neue Software zur Koregistrierung und Visualisierung von quantitativen PET-Perfusionsbildern mit der Koronarmorphologie aus einer CT-Angiographie vor.
Methodik
In unserer Software verwenden wir ein PET-Uptake-Bild für die Koregistrierung mit dem CT-Datensatz. Die Ergebnisse der Koregistrierung werden dann auf die parametrische Oberfläche aus der Kompartmentmodellierung übertragen. Um die Reproduzierbarkeit der manuellen Koregistrierung zu evaluieren, berechneten wir die Abweichung der Ergebnisse von fünf erfahrenen Untersuchern an neun Paaren unregistrierter PET und CT-Datensätze. Wir verwenden zweidimensionale Transferfunktionen, um die Koronarien aus einer CT-Angiographie im kombinierten Datensatz hervorzuheben.
Ergebnisse
Der mittlere Abstand im Raum betrug für drei Referenzpunkte zwischen 3,7 und 4,1 mm, der maximale Abstand 10,6 mm. Durch Einsatz der zweidimensionalen Transferfunktionen konnten die Koronarien problemlos in den kombinierten Datensätzen visualisiert werden.
Schlussfolgerungen
Mit der von uns vorgestellten Methode ist es möglich, eine quantitative Perfusions-PET kombiniert mit der Koronaranatomie aus einer CT-Angiographie darzustellen. Unsere ersten Ergebnisse zeigen, dass die manuelle Koregistrierung mit unserem Werkzeug reproduzierbar und eine kombinierte Visualisierung der kombinierten Datensätze in kurzer Zeit möglich ist.
Keywords: Coronary artery disease; CT angiography; cardiac PET; quantitative perfusion measurement; Koronare Herzerkrankung; CT-Angiographie; PET; quantitative Perfusionsmessung
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Zeitschrift für Medizinische Physik 19(2009), 182-188
DOI: 10.1016/j.zemedi.2009.05.005
ISSN: 0939-3889
Cited 5 times in Scopus
Downloads
Permalink: https://www.hzdr.de/publications/Publ-13226
Comparison of [18F]FDG uptake and distribution with hypoxia and proliferation in FaDu human squamous cell carcinoma (hSCC) xenografts after single dose irradiation
Bruechner, K.; Bergmann, R.; Santiago, A.; Mosch, B.; Yaromina, A.; Hessel, F.; Hofheinz, F.; van den Hoff, J.; Baumann, M.; Beuthien-Baumann, B.
Abstract
Purpose: This study investigated the uptake of [18F]2-fluoro-2-deoxy-glucose ([18F]FDG) in the human tumour xenograft FaDu at early time points after single dose irradiation with Positron-Emission-Tomography (PET), autoradiography and functional histology. Materials and methods: [18F]FDG-PET of FaDu hSCC xenografts on nude mice was performed before 25 Gy or 35 Gy single dose irradiation and one, seven or 11 days post irradiation (p.irr.). Before the second PET, mice were injected with pimonidazole (pimo) and bromodeoxyuridine (BrdU). After the PET tumours were excised, sliced and subjected to autoradiography and functional histology staining (pimo, BrdU, Ki67). [18F]FDG tumour uptake was quantified in the PET scans by maximal standard uptake value (SUVmax) and in the autoradiography after co-registration to the histology slices. Results: No differences in the overall [18F]FDG uptake between the two dose groups and time points were found with PET or autoradiography. Comparing!
autoradiography and histology, the [18F]FDG uptake was constant in tumour necrosis over time, while it decreased in vital tumour areas and particularly in hypoxic regions. No differences in the [18F]FDG uptake between positive and negative areas of Ki67 and BrdU were found. Conclusions: The decline of [18F]FDG uptake in vital tumour and in pimopositive areas as seen in autoradiography, was not reflected by evaluation of SUVmax determined by PET. These findings suggest that the SUVmax does not necessarily reflect changes in tumour biology after irradiation.
Keywords: Positron emission tomography; FDG; human tumour xenografts; single dose irradiation; hypoxia; proliferation
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International Journal of Radiation Biology 85(2009), 772-780
DOI: 10.1080/09553000903043067
ISSN: 0955-3002
Cited 16 times in Scopus
Permalink: https://www.hzdr.de/publications/Publ-13225
Synthesis and characterization of rhenium and technetium-99m tricarbonyl complexes bearing the 4-[3-bromophenyl]quinazoline moiety as a biomarker for EGFR-TK imaging
Bourkoula, A.; Paravatou-Petsotas, M.; Papadopoulos, A.; Santos, I.; Pietzsch, H.-J.; Livaniou, E.; Pelecanou, M.; Papadopoulos, M.; Pirmettis, I.
Abstract
Aiming at the development of technetium-99m (99mTc) complexes for early detection and staging of EGFR positive tumors, the tyrosine kinase inhibitor 6-amino-4-[(3-bromophenyl)amino]quinazoline was derivatized with pyridine-2-carboxaldehyde to generate the imine 6-(pyridine-2-methylimine)-4-[(3-bromophenyl) amino]quinazoline suitable for reacting with the fac-[99mTc(CO)3]+ core as an N,N bidentate ligand. The labelling was performed in high yield (>90%) by ligand exchange reaction using fac-[99mTc(OH2)3(CO)3]+ as precursor. The 99mTc complex was characterized by comparative HPLC analysis using the analogous rhenium (Re) complex as reference. The Re complex was prepared by ligand exchange reaction using the fac-[ReBr3(CO)3]2- as precursor and was fully characterized by NMR and IR spectroscopies and elemental analysis. In vitro studies indicate that both the ligand and its Re complex
inhibit the EGFR autophosphorylation (IC50: 17± 3.7 and 114 ± 23 nM respectively) in intact A431 cells, bind the receptor in a reversible mode, and inhibit A431 cell growth (IC50: 5.2 ± 1.1 and 2.0 ± 0.98 µM respectively). Biodistribution of the 99mTc complex in healthy animals showed a rather fast blood and soft tissue clearance between 1 and 15 min p.i. with excretion occurring mainly via the hepatobiliary system.
Keywords: Technetium; Rhenium; 4-Anilinoquinazoline; Tyrosine kinase inhibitors; Epidermal growth factor receptor
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European Journal of Medicinal Chemistry 44(2009), 4021-4027
DOI: 10.1016/j.ejmech.2009.04.033
Cited 43 times in Scopus
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Permalink: https://www.hzdr.de/publications/Publ-13224
Isomerism in tetrahedral rhenium cluster complexes [Re4Q4(PMe2sub>Ph)4X8]·nCH2Cl2 (Q = Se, X = Br; Q = Te, X = Cl, Br).
Efremova, O. A.; Mironov, Y. V.; Brylev, K. A.; Fedorov, V. E.; Pietzsch, H.-J.; Stephan, H.
Abstract
Three new tetrahedral rhenium cluster compounds [Re4Se4(PMe2Ph)4Br8].1.5CH2Cl2 (1), [Re4Te4(PMe2Ph) 4Br8].CH2Cl2 (2), and [Re4Te4(PMe2Ph)4Cl8].CH2Cl2 (3) have been synthesized by the reaction of the corresponding precursor chalcohalide complexes [Re4Q4(TeX2)4X8] (X = Br, Q = Se (for 1), Te (for 2); X = Cl, Q = Te (for 3)) with dimethylphenylphosphine in CH2Cl2. All compounds have been characterized by X-ray single-crystal diffraction and elemental analyses, IR and 31P NMR spectroscopy. 31P NMR spectroscopy indicates the formation of isomers in solution, confirmed by single-crystal X-ray analysis.
Keywords: Rhenium tetrahedral cluster complexes; Synthesis; Crystal structure; Isomerism; Organic ligands
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Polyhedron 28(2009), 2973-2976
DOI: 10.1016/j.poly.2009.07.003
Cited 3 times in Scopus
Permalink: https://www.hzdr.de/publications/Publ-13223
High-peak power diode-pumped Yb:CaF2 laser
Siebold, M.; Hornung, M.; Hein, J.; Reinhard, U.; Kaluza, M.
Abstract
Recent result of a 1 TW directly diode-pumped laser using Yb:Ca2 as amplifying medium.
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Lecture (Conference)
Conference on Lasers and Electro-Optics Europe (CLEO), 14.-19.06.2009, München, Deutschland
Permalink: https://www.hzdr.de/publications/Publ-13222
Gittersensortechnologie und ihr Einsatzpotenzial in der Chemieindustrie
Hampel, U.
Abstract
Die experimentelle Untersuchung von Mehrphasenströmungen erlangt eine zunehmende Bedeutung in der Optimierung chemischer und verfahrenstechnischer Prozesse sowie bei der Überprüfung thermohydraulischer Modelle für Mehrphasenströmungen. Zur Untersuchung von Flüssigkeitsströmungen mit und ohne Gasanteil wurden am Institut für Sicherheitsforschung des Forschungszentrums Dresden-Rossendorf Gittersensoren entwickelt, die eine schnelle Visualisierung der Phasenzusammensetzung von Stoffgemischen ermöglichen. Die Einsatzbreite von Gittersensoren in der Chemieindustrie reicht von der Überwachung und Prozesskontrolle in chemischen Reaktoren, wie Kolonnen, Säulenreaktoren und Rieselbettreaktoren, über die Mehrphasendurchflussmessung, bildgebende Füllstands- und Separationsmessung bis hin zur Validierung von Rechenmodellen für verfahrenstechnische Prozesse. Der Vortrag gibt einen Einlick in die Technologie sowie potenzielle Anwendungsfelder.
Keywords: wire mesh sensors; chemical engineering
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Lecture (others)
Seminar "Sensoranwendung in der Chemieindustrie" der BASF Ludwigshafen, 14.10.2009, Ludwigshafen, Germany
Permalink: https://www.hzdr.de/publications/Publ-13221
Wire mesh sensor technology - on the road towards three-phase flow measurement
Hampel, U.
Abstract
Wire mesh sensors are tools for ultrafast cross-sectional imaging of gas-liquid two-phase flows. They are helpful measurement devices for flow studies in fundamental chemical, nuclear and process engineering research problems, where multiphase flows play a role. A recent development of this technology is the capacitance wire-mesh sensor, which may be used to study phase fraction distributions in electrically non-conducting liquids. This is of particular importance for problems related to mineral oil processing. The presentation gives an overview on the current state-of-the-art in wire mesh sensor technology and discusses its potential for the studiy of complex and transient liquid-liquid-gas three-phase flows.
Keywords: wire mesh sensor; multiphase flow
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Invited lecture (Conferences)
Multiphase Club, 13.-14.10.2009, London, UK
Permalink: https://www.hzdr.de/publications/Publ-13220
High-efficiency, room-temperature nanosecond Yb:YAG laser
Siebold, M.; Loeser, M.; Schramm, U.; Koerner, J.; Wolf, M.; Hellwing, M.; Hein, J.; Ertel, K.
Abstract
Yb3+-doped gain media offer favorable properties for diode-pumped laser amplifiers for high-energy ns-pulses. To reach high optical-to-optical conversion efficiencies at room temperature however, very high and often impractical fluences are required both for pumping and extraction. Low temperature operation offers a solution, but the required cryogenic cooling systems add considerable complexity, bulkiness and cost. Multi-passing both pump and extraction beams through the gain medium is an alternative approach to overcome efficiency limitations at room temperature. In this article we present numerical and experimental results to this effect.We demonstrated ns-pulse output from a diode-pumped Yb:YAG amplifier at an energy of 566 mJ and an optical-to-optical efficiency of 20 %, which is almost a doubling of the efficiency achieved with ns-lasers employing Yb3+-doped gain media at this energy level.
Keywords: Laser amplifiers; Lasers ytterbium: Lasers diode-pumped
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Optics Express 17(2009)22, 19887-19893
DOI: 10.1364/OE.17.019887
Cited 22 times in Scopus
Permalink: https://www.hzdr.de/publications/Publ-13219
Synthesis of Benzoate-Functionalized Phosphanes as Novel Building Blocks for the Traceless Staudinger Ligation
Mamat, C.; Flemming, A.; Köckerling, M.; Steinbach, J.; Wuest, F.
Abstract
A new synthetic pathway for the preparation of benzoate-functionalized phosphanes for microwave-mediated traceless Staudinger ligations is described. Novel phosphane derivatives based on 4-substituted iodophenyl benzoates were prepared via palladium(II)-catalyzed PC cross-coupling reaction strategy in high yields. The application of microwave conditions for the ligation reactions reduced the reaction time considerably. An approach to fast and facile labeling strategies using this ligation was established.
Keywords: Staudinger ligation; traceless; click chemistry; PC cross-coupling; palladium-catalyzed
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Synthesis 19(2009), 3311-3321
DOI: 10.1055/s-0029-1216947
Cited 26 times in Scopus
Permalink: https://www.hzdr.de/publications/Publ-13218
Reduction of Arteriosclerotic Nanoplaque Formation and Size by n-3 Fatty Acids in Patients after Valvular Defect Operation
Koppe, C.; Rodriguez, M.; Winkler, K.; Pietzsch, J.; Neumann, K.; Hiemann, N. H.; Hetzer, R.; Malmsten, M.; Siegel, G.
Abstract
Summary
Background/Methods: Coating a silica surface with the isolated lipoprotein receptor heparan sulfate proteoglycan (HS-PG) from arterial endothelium and vascular matrices, we could observe the very earliest stages of arteriosclerotic plaque development by ellipsometric techniques in vitro (patent EP 0 946 876). This so-called nanoplaque formation is represented by the ternary aggregational complex of the HS-PG receptor, lipoprotein particles and calcium ions. The model was validated in several clinical studies on statins in cardiovascular high-risk patients applying their native blood lipoprotein fractions.
Results: In 7 patients who had undergone a valvular defect operation, the reduction of arteriosclerotic nanoplaque formation in normal Krebs solution amounted to 6.1 ± 2.3% (p < 0.0156) and of nanoplaque size to 37.5 ± 13.2% (p < 0.0312), respectively, after a 3-month therapy with n-3 fatty acids (3 × 3 g daily, Ameu® 500 mg). Additionally, the quotient oxLDL/LDL was lowered by 6.8 ± 2.1% (p < 0.0166), the MDA concentration remained unchanged and the lipoprotein(a) concentration decreased by 15.8 ± 5.6% (p < 0.0469) in the patients blood. The concentration of the nanoplaque promoting particles VLDL and total triglycerides was diminished by 34.1 ± 11.6% (p < 0.0469) and 26.7 ± 10.8% (p < 0.0156), respectively. Furthermore, the ratio of the strongly atherogenic small dense to the total LDL cholesterol (LDL5+LDL6)/LDLtot decreased by 9.9 ± 3.0% (p < 0.0174).
Conclusions: A combinatorial regression analysis revealed a basis for a mechanistic explanation of nanoplaque reduction under n-3 fatty acid treatment. This effect was possibly due to the beneficial changes in lipid concentrations and an attenuation of the risk factors oxLDL/LDL and (LDL5+LDL6)/LDLtot.
Zusammenfassung
Hintergrund/Methode: Durch Beschichtung einer Silikatoberfläche mit dem Lipoproteinrezeptor Heparansulfat-Proteoglykan (HS-PG), der aus arteriellem Endothel und der Gefäßmatrix isoliert wurde, konnten wir mithilfe ellipsometrischer Techniken die ersten Anfangsstadien arteriosklerotischer Plaques in vitro beobachten (Patent EP 0 946 876). Die sogenannten Nanoplaques werden durch den ternären Aggregatkomplex aus HS-PGRezeptor, Lipoproteinpartikeln und Kalziumionen gebildet. Das Modell wurde in mehreren klinischen Studien zur Wirkung von Statinen bei kardiovaskulären Hochrisikopatienten bestätigt, wobei deren natürliche Blut-Lipoprotein-Fraktionen eingesetzt wurden.
Ergebnisse: Bei 7 Patienten nach Herzklappenoperation betrug die Reduktion der arteriosklerotischen Nanoplaquebildung und -größe nach 3-monatiger Therapie mit ω-3-Fettsäuren (3 × 3 g/d Ameu® 500 mg) in normaler Krebslösung 6,1 ± 2,3% (p < 0,0156) bzw. 37,5 ± 13,2% (p < 0,0312). Zusätzlich wurde im Patientenblut der oxLDL/LDL-Quotient um 6,8 ± 2,1% (p < 0,0166) gesenkt, die MDA-Konzentration blieb unverändert und die Lipoprotein(a)-Konzentration nahm um 15,8 ± 5,6% (p < 0,0469) ab. Die Konzentration der Nanoplaque fördernden VLDLs und Gesamttriglyzeride wurde um 34,1 ± 11,6% (p < 0,0469) sowie 26,7 ± 10,8% (p < 0,0156) reduziert. Ferner verringerte sich das Verhältnis der stark atherogenen, kleinen dichten LDL-Fraktionen zum Gesamt-LDL (LDL5+LDL6)/LDLtot um 9,9 ± 3,0% (p < 0,0174).
Schlussfolgerungen: Eine mehrfache Regressionsanalyse ergab eine Grundlage für eine mechanistische Erklärung der Nanoplaquereduktion unter ω-3-Fettsäure-Behandlung. Dieser Effekt beruht möglicherweise auf günstigen Veränderungen der Lipidkonzentrationen und einer Verminderung der Risikofaktoren oxLDL/LDL und (LDL5+LDL6)/LDLtot.
Keywords: Proteoglycan receptor; Lipoproteins; Nanoplaque formation; n-3 Fatty acids; Clinical trial; Proteoglykanrezeptor; Lipoproteine; Nanoplaquebildung; ω-3-Fettsäuren; Klinische Studie
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Forschende Komplementärmedizin / Research in Complementary Medicine 16(2009), 237-245
DOI: 10.1159/000229786
Cited 3 times in Scopus
Permalink: https://www.hzdr.de/publications/Publ-13217
Direct labelling of peptides with 2-[F-18]fluoro-2-deoxy-D-glucose ([F-18]FDG)
Wuest, F.; Hultsch, C.; Berndt, M.; Bergmann, R.
Abstract
The study describes the use of [F-18]FDG as F-18 building block for the direct labelling of various aminooxy-functionalised peptides via chemoselective oxime formation.
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Bioorganic & Medicinal Chemistry Letters 19(2009), 5426-5428
DOI: 10.1016/j.bmcl.2009.07.108
ISSN: 0960-894X
Cited 43 times in Scopus
Permalink: https://www.hzdr.de/publications/Publ-13216
Properties of Transparent Conductive Oxides Deposited by Magnetron Sputtering
Vinnichenko, M.; Cornelius, S.; Rogozin, A.; Shevchenko, N.; Gago, R.; Kolitsch, A.; Möller, W.
Abstract
Transparent conductive oxides (TCOs) are attracting an increasing attention as materials for transparent electrodes in thin film solar cells. The characteristic features of TCOs are low formation energy of defects, which enables n-type doping, and low probability of compensating defects formation. These materials are mainly based on In2O3, SnO2 and ZnO, wide band gap (>3 eV) semiconductors, which may be easily converted by doping to degenerate semiconductors with electrical resistivity as low as ~10-4 Ohm cm and high transmittance (>80%) in the visible spectral range. In addition to these properties, photovoltaic applications require TCO materials with increased near-IR transmittance, adjustable work function and defined surface morphology, which improves light trapping in PV absorber layer (e.g. a-Si:H-based cells). The need to decrease TCO production costs has stimulated research activity on reactive pulsed magnetron sputtering (RPMS) as a versatile deposition method.
In order to explore potential advantages of RPMS, the relationship between the deposition parameters and structure, phase composition, and physical properties of TCOs should be established. Understanding the mechanisms of donor impurity incorporation and its electrical activation is of special importance. For this purpose, indium oxide (IO), ITO, ZnO, and AZO films (with Al concentrations 0.7-8.7 at. %) were grown by RPMS with a precise control of the oxygen partial pressure at substrate temperatures ranging from ~40 °C to 580 °C. The magnetron plasma parameters were determined by a Langmuir probe. The resulting films were characterized by spectroscopic ellipsometry, Hall effect measurements, X-ray diffraction (XRD) and, in case of ZnO and AZO films, by X-ray absorption near edge spectroscopy (XANES). The Sn concentration in ITO was determined by Auger analysis, while the Al concentration in ZnO matrix was estimated by elastic recoil detection analysis.
The comparison of the real-time behavior of the IO and ITO film structure and electrical properties during annealing provides a direct evidence of Sn donor activation (with an estimated efficiency of 40%) in ITO due to amorphous-to-crystalline transition. The ITO film crystallinity always improves with increasing substrate temperature or during isothermal annealing, with the electrical resistivity decreasing. In contrast, the electrical resistivity of ZnO:Al films shows a clear minimum at a certain substrate temperature (250-400 °C), which depends on Zn/O2 flux ratio and correlates with a maximum in crystallinity (grain size). In this case, the highest mobility value of 46 cm2 V-1 s-1 is comparable to the best values achieved in AZO films grown by less cost-efficient techniques. This value is achieved at the free electron density of 6x1020 cm-3 which corresponds to maximum ~30% electrical activation of Al impurity. At higher temperatures, the AZO electrical properties and crystalline quality deteriorate abruptly. This is likely due to formation of a new metastable phase, which is identified by XANES as homologous (ZnO)3(Al2O3). Its formation is triggered by an increase of the Al/Zn ratio in the film, and leads to electrical deactivation of the Al impurity in AZO. In order to improve electrical activation of the donor impurity and to extend the functionality of TCOs, the formation of epitaxial AZO and TiO2:Nb films by RPMS is proposed.
Keywords: transparent conductive oxides; Al-doped ZnO; tin-doped indium oxide
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Invited lecture (Conferences)
16th International Summer School on Vacuum, Electron and Ion Technologies (VEIT 2009), 28.09.-02.10.2009, Sunny Beach, Bulgaria
Permalink: https://www.hzdr.de/publications/Publ-13215
Radiopharmacological investigation of 3-[4-[F]fluorobenzylidenyl]-indolin-2-one
Bergmann, R.; Knieß, T.; Kuchar, M.; Steinbach, J.; Wüst, F.
Abstract
Introduction and Aim:
The radiopharmacological evaluation of the new compound 3-[4-[18F]fluorobenzylidenyl]-indolin-2-one is described. The compound is a radiolabeled derivative of an inhibitor of the VEGF-mediated signaling through the Flk-1/KDR (VEGFR-2) tyrosine kinase receptor pathway (SU5416 (NSC 696819) [3-(3,5-dimethyl-1H-pyrrol-2-ylmethylene)-1,3-dihydro-indol-2-one]).
Materials and Methods:
The radiosynthesis was accomplished by Knoevenagel condensation of 4-[18F]fluorobenzaldehyde with oxindole in a remotely controlled synthesis module. The radiotracer was obtained after a two-step labeling procedure in 4% decay-corrected radiochemical yield at a specific activity of 48-61 GBq/µmol within 90 min. The radiochemical purity after semi-preparative HPLC purification exceeded 98%. The biodistribution, metabolism and excretion were studied in Wistar rats. Small animal PET studies in rats and FaDu tumor bearing nude mice were carried out. Results: After distribution the radiotracer was rapidly accumulated in the adrenals, liver and kidneys, however, it was cleared from these and the most other organs. Only the adipose tissue retained the activity over 60 min. Unexpected high transient uptake was observed in the brain, pancreas, heart and lung. The fast blood clearance of 3-[4-[18F]fluorobenzylidenyl]-indolin-2-one was caused by excretion, approximately one half each was renal and biliary excreted and other metabolic processes. Only the original compound was entering the brain. In arterial blood plasma were two more polar radiometabolites detected. The blood clearance was fast and could be described by a two phase elimination with half-lifes of 8 and 267 s. Consequently, in small animal PET studies with FaDu tumor bearing mice - no specific uptake in the tumors could be detected.
Conclusion:
The investigation of the 3-[4-[18F]fluorobenzylidenyl]-indolin-2-one revealed that the uptake in high perfused organs was transiently, and only in the adipose tissue the compound was accumulated. However, it seems to be it is not applicable for angiogenesis imaging.
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Poster
World Molecular Imaging Congress 2009, 23.-26.09.2009, Montreal, Canada
Permalink: https://www.hzdr.de/publications/Publ-13214
Cell uptake studies of fluorescent labeled phophopeptide-cell-penetrating peptide hybrids
Richter, S.; Bergmann, R.; Neundorf, I.; Beck-Sickinger, A.; Pietzsch, J.; Steinbach, J.; Wüst, F.
Abstract
Introduction and Aim:
Phosphopeptides are very useful reagents to study signal transduction pathways related with cellular protein phosphorylation/dephosphorylation processes. Phosphopeptides also have been identified as important drug candidates to modulate intracellular signal transduction pathways. The present study describes the use of cell-penetrating peptides (CPPs) sC18 and hCT(18-32)-k7 coupled to Polo-like kinase-1 (Plk-1)-binding hexaphosphopeptide H-Met-Gln-Ser-pThr-Pro-Leu-OH to investigate cell uptake of the corresponding phosphopeptide-CPP hybrids.
Materials and Methods:
Peptide syntheses were accomplished using a combination of automated and manual solid-phase peptide syntheses following standard Fmoc chemistry. Fluorescence labeling was carried out via coupling 5(6)-carboxyfluoresceine (CF) to the N-terminal end of the phosphopeptide using HATU as the activation agent, DIPEA as the base, and DMF as the solvent. Cell uptake studies of CF-Met-Gln-Ser-pThr-Pro-Leu-sC18 (CF-I) and CF-Met-Gln-Ser-pThr-Pro-Leu-hCT(18-32)-k7 (CF-II) were performed using the human breast cancer cell line MCF-7 and human cervical carcinoma epithelial (HeLa) cells on a Zeiss Axio fluorescence confocal microscope. Results: Peptide hybrids CF-I and CF-II showed cellular uptake in both cell lines after incubation at 37°C for 60 min. Cell uptake was more pronounced in HeLa cells compared to MCF-7 cells. Phosphopeptide conjugated to sC18 showed higher cell uptake compared to phosphopeptide-hCT(18-32)-k7 conjugate. As expected, CF-labeled phosphopeptide without being conjugated to CPPs as molecular shuttles was not internalized into both cell lines. Quantification of cellular uptake using flow cytometry analysis and fluorine-18 labeled phosphopeptide-CPP hybrids are currently in progress.
Conclusion:
Cell-penetrating peptides sC18 and hCT(18-32)-k7 are useful drug delivery systems enabling sufficient membrane transport of phosphopeptides to further promote studies on intracellular metabolic pathways involving phosphopeptides.
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Poster
World Molecular Imaging Congress 2009, 23.-26.09.2009, Montreal, Canada
Permalink: https://www.hzdr.de/publications/Publ-13213
Deep Subthreshold Xi- Production in Ar+KCl Reactions at 1.76A GeV
Agakishiev, G.; Balanda, A.; Bassini, R.; Belver, D.; Belyaev, A. V.; Blanco, A.; Böhmer, M.; Boyard, J. L.; Braun-Munzinger, P.; Cabanelas, P.; Castro, E.; Chernenko, S.; Christ, T.; Destefanis, M.; Díaz, J.; Dohrmann, F.; Dybczak, A.; Eberl, T.; Fabbietti, L.; Fateev, O. V.; Finocchiaro, P.; Fonte, P.; Friese, J.; Fröhlich, I.; Galatyuk, T.; Garzón, J. A.; Gernhäuser, R.; Gil, A.; Gilardi, C.; Golubeva, M.; González-Díaz, D.; Guber, F.; Hennino, T.; Holzmann, R.; Iori, I.; Ivashkin, A.; Jurkovic, M.; Kämpfer, B.; Kanaki, K.; Karavicheva, T.; Kirschner, D.; Koenig, I.; Koenig, W.; Kolb, B. W.; Kotte, R.; Krizek, F.; Krücken, R.; Kühn, W.; Kugler, A.; Kurepin, A.; Lang, S.; Lange, J. S.; Lapidus, K.; Liu, T.; Lopes, L.; Lorenz, M.; Maier, L.; Mangiarotti, A.; Markert, J.; Metag, V.; Michalska, B.; Michel, J.; Mishra, D.; Morinière, E.; Mousa, J.; Müntz, C.; Naumann, L.; Otwinowski, J.; Pachmayer, Y. C.; Palka, M.; Parpottas, Y.; Pechenov, V.; Pechenova, O.; Pietraszko, J.; Przygoda, W.; Ramstein, B.; Reshetin, A.; Roy-Stephan, M.; Rustamov, A.; Sadovsky, A.; Sailer, B.; Salabura, P.; Schmah, A.; Sobolev, Y. G.; Spataro, S.; Spruck, B.; Ströbele, H.; Stroth, J.; Sturm, C.; Sudol, M.; Tarantola, A.; Teilab, K.; Tlusty, P.; Traxler, M.; Trebacz, R.; Tsertos, H.; Wagner, V.; Weber, M.; Wisniowski, M.; Wojcik, T.; Wüstenfeld, J.; Yurevich, S.; Zanevsky, Y. V.; Zhou, P.; Zumbruch, P.
Abstract
We report first results on a deep subthreshold production of the doubly strange hyperon Xi- in a heavy-ion reaction. At a beam energy of 1.76A GeV the reaction Ar+KCl was studied with the High Acceptance Di-Electron Spectrometer at SIS18/GSI. A high-statistics and high-purity Lambda sample was collected, allowing for the investigation of the decay channel Xi--->Lambdapi-. The deduced Xi-/(Lambda+Sigma0) production ratio of (5.6±1.2-1.7
+1.8)×10-3 is significantly larger than available model predictions.
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Physical Review Letters 103(2009), 132301
DOI: 10.1103/PhysRevLett.103.132301
Cited 86 times in Scopus
Permalink: https://www.hzdr.de/publications/Publ-13212
Quantum oscillations in the normal and superconducting state of LuNi2B2C
Bergk, B.; Maniv, T.; Zhuravlev, V.; Canfield, P. C.; Wosnitza, J.
Abstract
We present de Haas-van Alphen (dHvA) investigations in the nonmagnetic borocarbide superconductor LuNi2B2C both in the normal and in the superconducting state. The measurements have been carried out by use of the torque method as well as by the field-modulation method. The quantum oscillations in the normal state give information on the elaborated Fermi surfaces which consists of several open and closed parts [1]. In the superconducting state we observe dHvA oscillations that belong to a spheroidal Fermi surface deep into the superconducting state down to B = 2.5 T far below the upper critical field, Bc2. We find only a minor additional damping of the dHvA oscillation amplitude in the superconducting state compared to the normal state. Only close to Bc2 the oscillations appear to be more strongly damped. There, the background signal shows a strong peak effect which complicates the analysis of the dHvA signal in this region. However, the apparent increase of the additional damping in the peak-effect range hints at the influence of increased flux-line pinning in this region
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Poster
9th International Conference on Materials and Mechanisms of Superconductivity (M2S-IX), 07.-12.09.2009, Tokyo, Japan
Permalink: https://www.hzdr.de/publications/Publ-13211
Magnetic Order and Magnetic Exchange Interactions in the Quasi-Two-Dimensional Magnets [Cu(pyz)2(HF2)]X with X = BF4 and PF6
Wosnitza, J.; Beyer, R.; Cizmar, E.; Ozerov, M.; Skourski, Y.; Uhlarz, M.; Zvyagin, S. A.; Gemming, S.; Sengupta, P.; Batista, C.; Schlueter, J. A.; Manson, J. L.
Abstract
We report on combined experimental and theoretical efforts to elucidate the magnetic properties of the organic magnets [Cu(HF2)(pyz)2]X with X = BF4 and PF6. By use of high-resolution specific-heat measurements on high-quality single crystals we were able to resolve small lambda-type anomalies indicative for a phase transition into a long-range ordered state. First-principles density-functional calculations allow to estimate the exchange couplings and confirm a three-dimensional antiferromagnetic order between ad-jacent Cu centers with a stronger coupling within the layers of pyz-bridged Cu and a much weaker cou-pling across the HF2 linker units. Specific-heat data in magnetic field, B,reveal a slightly anisotropic nonmonotonic dependence of the Néel temperature TN with B. The increase of TN at low fields can be un-derstood by the reduction of phase fluctuations that are prominent in these highly anisotropic quasi-two-dimensional magnets. Towards higher fields, B suppresses the amplitude of the antiferromag-netic order parameter, and correspondingly TN, by aligning the spins parallel to B. This nonmonotonic be-havior of TN, as well as the magnetic part of the specific heat, cannot be described by a mean field theory that neglects the crucial role played by phase fluctuations. In contrast, we show that both properties are very well reproduced by Quantum Monte Carlo simulations. Pulsed-field magnetization data corroborate the strong anisotropy of the exchange interactions. The ratio of the inter- to intralayer exchange interac-tion is estimated as 0.0025 (for X = BF4) and 0.009 (X = PF6). High-field electron spin resonance meas-urements reveal a magnetic easy-plane anisotropy.
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Invited lecture (Conferences)
The 8th International Symposium on Crystalline Organic Metals, Superconductors and Ferromagnets (ISCOM 2009), 12.-17.09.2009, Hokkaido, Japan
Permalink: https://www.hzdr.de/publications/Publ-13210
Magnetic quantum oscillations in borocarbide superconductors
Bergk, B.; Wosnitza, J.
Abstract
We report systematic de Haasvan Alphen (dHvA) investigations in the normal and superconducting state of RNi2B2C (R = Y and Lu). The observed rich frequency spectrum of the dHvA signals results from a rather complex electronic band structure with different open and closed Fermi-surface sheets. From our data in combination with full-potential local-orbital calculations we are able to extract the angular-resolved mass-enhancement factors, lambda, for different bands. We find a strong anisotropy and band dependence of lambda, clearly reflecting the multiband character of the superconductivity in RNi2B2C. We further were able to resolve dHvA oscillations deep into the superconducting state. The observed additional damping of the dHvA amplitudes is much less than expected from most theories. This hints at a reduced or even zero superconducting gap for the detected Fermi surface
- Low Temperature Physics 35(2009)8/9, 872-878
Downloads
Permalink: https://www.hzdr.de/publications/Publ-13209
Status of the Umbrella project LONGLIFE
Altstadt, E.
Abstract
In view of the increasing age of the European NPPs and envisaged life time extensions up to an EOL of 80 years, there is a need for an improved understanding and prediction of RPV irradiation embrittlement effects connected with long term operation (LTO). Effects caused by high neutron fluences such as the possible formation of Late Blooming Phases and as yet unknown defects must be considered adequately in safety assessments. However, the surveillance database for long irradiation times (>20 years) and low neutron flux is sparse, which leads to uncertainties in the treatment of LTO irradiation effects. In this context microstructural data are essential for the understanding of the involved mechanisms. The proposed project aims at: 1) improved knowledge on LTO phenomena relevant for European reactors; 2) assessment and proposed improvements of prediction tools, codes and standards; 3) elaboration of best practice guidelines for irradiation embrittlement surveillance.
The suggested scope of work is:
i) Summary of boundary conditions for LTO and systematic (re)evaluation of the international prediction procedures of irradiation embrittlement
ii) Generation of microstructural data of irradiated representative or original RPV materials; demonstration that damage models are (or not) consistent with the mechanisms of irradiation damage in the LTO (use of PERFORM60 prediction tools)
iii) Investigation of specific LTO relevant phenomena like late blooming phases and flux effect from available results; role of Cu, Ni, Mn, P, Si under the aspect of LTO;
iv) Correlation of microstructural data with mechanical properties and identification of the most important influencing factors (link with PERFORM60)
v) Influence of high neutron fluences on fracture toughness curves shape
vi) Comparison of embrittlement results from decommissioned plants with surveillance data
vii) Elaboration of recommendations for RPV embrittlement surveillance under LTO conditions
Keywords: Reactor Pressure Vessel; Irradiation defects; Long term operation; FP7 Project
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Lecture (others)
5-th NULIFE Network meeting, 15.-17.09.2009, Les Renardieres, France
Permalink: https://www.hzdr.de/publications/Publ-13208
KKW Krümmel Ermüdungsbeitrag der Transiente vom 28.06.2007 für den RDB-Boden
Altstadt, E.
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Article, self-published (no contribution to HZDR-Annual report)
Forschungszentrum Rossendorf 2009
FZD\FWS\2009\04
18 Seiten
ISSN: 1437-322X
Permalink: https://www.hzdr.de/publications/Publ-13207
Mechanische Analyse für die RDB-Deckel-Verbindung des Kernkraftwerks Brunsbüttel
Altstadt, E.; Werner, M.
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Article, self-published (no contribution to HZDR-Annual report)
Forschungszentrum Rossendorf 2009
FZD\FWS\2009\05
22 Seiten
ISSN: 1437-322X
Permalink: https://www.hzdr.de/publications/Publ-13206
VVER vessel steel corrosion at interaction with molten corium in oxidizing atmosphere
Bechta, S. V.; Granovsky, V. S.; Khabensky, V. B.; Krushinov, E. V.; Vitol, S. A.; Sulatsky, A. A.; Gusarov, V. V.; Almiashev, V. I.; Lopukh, D. B.; Bottomley, D.; Fischer, M.; Piluso, P.; Miassoedov, A.; Tromm, W.; Altstadt, E.; Fichot, F.; Kymalainen, O.
Abstract
The long-term in-vessel corium retention (IVR) in the lower head bears a risk of the vessel wall deterioration caused by steel corrosion. The ISTC METCOR Project has studied physicochemical impact of prototypic coria having different compositions in air and steam and has generated valuable experimental data on vessel steel corrosion. It is found that the corrosion rate is sensitive to corium composition, but the composition of oxidizing above-melt atmosphere (air, steam) has practically no influence on it. A model of the corrosion process that integrates the experimental data, is proposed and used for development of correlations.
Keywords: Corium-steel interaction; in-vessel melt retention; physiochemical properties
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Nuclear Engineering and Design 239(2009), 1103-1112
DOI: 10.1016/j.nucengdes.2008.12.009
Cited 16 times in Scopus
Permalink: https://www.hzdr.de/publications/Publ-13205
Studying the astrophysical r-process: Multigap resistive plate chamber prototypes for NeuLAND
Abstract
At the future Facility for Antiproton and Ion Research (FAIR) in Darmstadt, Germany, uniquely intensive beams of radioactive ions will become available. One of the experiments at FAIR, called Reactions with Relativistic Radioactive Beams (R3B), will study reactions of such projectiles at energies up to 1 GeV/A. The planned NeuLAND time-of-flight detector will detect the emitted neutrons with a time resolution of sigma = 50 ps and efficiency of better than 90 %. The poster will discuss recent progress in the development of multigap resistive plate chamber based prototypes for NeuLAND. Using the ELBE electron beam facility in Dresden, the time resolution of the prototypes has been shown to fulfill the design criteria.
Keywords: Nuclear astrophysics; neutron time-of-flight; detector multigap; resistive plate chamber; MRPC; NeuLAND; R3B; FAIR
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Poster
Nuclear Physics in Astrophysics IV, 08.-12.06.2009, Frascati, Italien
Permalink: https://www.hzdr.de/publications/Publ-13204
The sorption processes of Np(V) and U(VI) onto metal oxide phases. The formation of sorption complexes and mechanistic aspects studied by in situ ATR FT-IR spectroscopy
Foerstendorf, H.; Müller, K.; Heim, K.
Abstract
The migration behaviour of actinide ions in the geosphere is generally influenced by sorption processes in aqueous media. These processes occurring at solid/liquid interfaces can be monitored by in situ Attenuated Total Reflection Fourier-transform Infrared (ATR FT-IR) spectroscopy providing structural information on a molecular level.[1]
In this work, the sorption of neptunium(V) onto metal oxides was investigated for the first time. From the Np(V) sorption studies on the metal oxides, stable surface species of NpO2+ are derived. The type of the sorbed species can be elucidated by a spectral shift (~ 30 cm−1) to lower wavenumbers of the antisymmetric stretching vibration υ3(NpO2+) compared to the aqueous species suggesting an inner-sphere complexation. Outer-sphere complexation is found to play a minor role due to the pH independence of the sorption species throughout the pH range 4 7.6. The comparative spectroscopic experiments of Np(V) sorption onto TiO2, SiO2 and ZnO indicate structurally similar bidentate surface complexes.[2]
A detailed insight into the molecular mechanisms occurring during the formation of ternary actinide complexes at the solid/liquid interface is provided upon formation of uranyl carbonato complexes on ferrihydrite (Fh). The influence of the presence of atmospheric carbon dioxide during the sorption processes of the actinide ions was studied by sorption experiments which were carried out under inert gas conditions and in an ambient atmosphere. From the results, the formation of bidentate [FhUO2O2CO] complexes can be derived under mildly acid conditions which is in agreement from recent EXAFS results obtained from batch samples.[3]
Furthermore, experiments with 13C labelled carbonate provide an unequivocal assignment of the spectral features reflecting the structural alterations of the carbonate ions upon sorption of uranyl cations onto Fh. From these assignments, the formation of the ternary uranyl complexes can be described at a molecular level.
References
[1] Lefèvre, G. (2004) Adv. Colloid Interface Sci. 107, 109-123.
[2] Müller, K. et al. (2009) Environ. Sci. Technol., in press.
[3] Rossberg, A. et al. (2009) Environ. Sci. Technol. 43, 1400-1406.
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Contribution to proceedings
16th Radiochemical Conference, 18.-23.04.2010, Marianske Lazne, Czech Republic
Chemicke listy, Vol. 104, Praha: Czech Chemical Society, 0009-2770, s178-s178 -
Lecture (Conference)
RadChem 2010 - 16th Radiochemical Conference, 18.-23.04.2010, Mariánske Lázne, Czech Republic
Permalink: https://www.hzdr.de/publications/Publ-13203
Enhancement Of Electrical And Chemical Surface Properties Of Titanium And Iron-Carbon Alloys Irradiated With A Low-Energy Intense Pulsed Electron Beam
Markov, A. B.; Reuther, H.; Shevchenko, N.; Kolitsch, A.
Abstract
Processes leading to homogenization of chemical and phase composition of near-surface layers materials made from titanium and iron-carbon alloys under irradiation of a low energy intense pulsed electron beam have been investigated. It has been shown that preliminary heating leads to appearance of a more homogeneous chemical composition of surface alloy. It has been determined that an electron-beam polishing took place during irradiation. Irradiation results in dissolution of secondary phase inclusions, decreasing of roughness, and as a result in the enhancement of electrical and chemical surface properties of titanium and iron-carbon alloys.
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Contribution to proceedings
19th Int. Crimean Conference Microwave & Telecommunication Technology, 14.-18.09.2009, Sevastopol, Ukraine
Enhancement Of Electrical And Chemical Surface Properties Of Titanium And Iron-Carbon Alloys Irradiated With A Low-Energy Intense Pulsed Electron Beam, 978-966-335-244-594 2., 593-594
Permalink: https://www.hzdr.de/publications/Publ-13202
Phase-sensitive terahertz spectroscopy with BWOs in reflection mode
Pronin, A. V.; Goncharov, Y. G.; Fischer, T.; Wosnitza, J.
Abstract
We report on a method, which allows accurate measurements of complex reflection coefficient of a solid at frequencies 1 to 50 cm-1 (30 GHz - 1.5 THz). Backward-wave oscillators (BWOs) are used as sources of monochromatic coherent radiation, tunable in frequency. The amplitude of the complex reflection (the reflectivity) is measured in a standard way, while the phase shift, introduced by the reflection from the sample surface, is measured using a polarizing Michelson interferometer. This method is particular useful for not-transparent samples (such as metals, superconductors, etc.), where phase-sensitive transmission measurements are not possible.
The method requires no Kramers-Kronig transformation in order to extract the sample's electrodynamic properties (such as complex dielectric function or complex conductivity). Another area of application of this method is the study of magnetic materials with complex dynamic permeability different from unity at the measurement frequencies (for example, metamaterials). Measuring both, the phase-sensitive transmission and the phase-sensitive reflection, would allow a straight-forward model-independent determination of the dielectric permittivity and magnetic permeability of such materials.
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Poster
The 34th International Conference on Infrared, Millimeter, and Terahertz Waves, 21.-25.09.2009, Busan, Korea
Permalink: https://www.hzdr.de/publications/Publ-13201
Memory effect of Mn5Ge3 nanomagnets embedded inside a Mn-diluted Ge matrix
Zhou, S.; Shalimov, A.; Potzger, K.; Helm, M.; Fassbender, J.; Schmidt, H.
Abstract
Crystalline Mn5Ge3 nanomagnets are formed inside a Mn-diluted Ge matrix using Mn ion implantation. A temperature-dependent memory effect and slow magnetic relaxation are observed below the superparamagnetic blocking temperature of Mn5Ge3. Our findings corroborate that the observed spin-glass-like features are caused by the size distribution of Mn5Ge3 nanomagnets, rather than by the inter-particle interaction through the Mn-diluted Ge matrix.
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Applied Physics Letters 95(2009), 192505
DOI: 10.1063/1.3264076
Cited 16 times in Scopus
Permalink: https://www.hzdr.de/publications/Publ-13200
Bruchmechanische Werkstoffcharakterisierung zur Überwachung der Neutronenversprödung von Reaktordruckbehältern für den Langzeitbetrieb von Kernkraftwerken
Zurbuchen, C.; Viehrig, H.-W.
Abstract
Die Schweizer Richtlinie HSK-AN-425 dient der bruchmechanische Werkstoffcharakterisierung zur Überwachung der Neutronenversprödung von Reaktordruckbehältern für den Langzeitbetrieb von Kernkraftwerken. Eine Besonderheit ist, dass nicht quasistatische, sondern dynamische Bruchzähigkeitskennwerte ermittelt werden. Die Richtlinie deckt den gesamten Bereich der Zähigkeit ferritischer Stähle ab, also vom instabilen Spaltbruch in der Tieflage (tiefe Temperaturen) bis zum duktilen Reissen in der Hochlage (hohe Temperaturen) und dem dazwischen liegenden Bereich des Steilabfalls der Zähigkeit.
Ziel des Forschungsprojektes HSK-AN-6305 war, die zentralen Elemente der neuen Richtlinie HSK-AN-425 Rev. 5 durch experimentelle Überprüfung an vergleichbaren Werkstoffen aus dem RDB Biblis C zu validieren (Einfluss der Risslänge, Fortsetzung der MC im oberen ZSÜ-Bereich). Allfällige Schwachstellen der Richtlinie HSK-AN-425 sind zu korrigieren, bevor sie in der Überwachung der Kernanlagen freigegeben werden kann. Der Einfluss der Probendicke und der Probenart auf die quasistatische MC-Referenztemperatur T0 nach ASTM E 1921 sowie auf die dynamische MC-Referenztemperatur T0d nach HSK-AN-425 ist zu bestimmen (Übertragbarkeit der Ergebnisse auf Bauteile und Komponenten), und ob bei den Bruchmechanikproben der herkömmliche Ermüdungsanriss durch EDM-Kerben ersetzbar ist.
In dieser Publikation werden die Ergebnisse des Forschungsprojektes HSK-AN-6305 ausführlich vorgestellt.
Keywords: fracture mechanics; quasistatic; dynamic; Master Curve; crack growth resistance curve; R curve; ASTM E 1921; ASTM E 1820; NM method; HSK-AN-425; HSK AN 425; stretch zone
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Article, self-published (no contribution to HZDR-Annual report)
Forschungszentrum Rossendorf 2009
FZD\FWS\2009\07
166 Seiten
ISSN: 1437-322X
Permalink: https://www.hzdr.de/publications/Publ-13199
Bruchmechanische Werkstoffcharakterisierung zur Überwachung der Neutronenversprödung von Reaktordruckbehältern für den Langzeitbetrieb von Kernkraftwerken- Kurzfassung
Zurbuchen, C.
Abstract
Die Schweizer Richtlinie HSK-AN-425 dient der bruchmechanische Werkstoffcharakterisierung zur Überwachung der Neutronenversprödung von Reaktordruckbehältern für den Langzeitbetrieb von Kernkraftwerken. Eine Besonderheit ist, dass nicht quasistatische, sondern dynamische Bruchzähigkeitskennwerte ermittelt werden. Die Richtlinie deckt den gesamten Bereich der Zähigkeit ferritischer Stähle ab, also vom instabilen Spaltbruch in der Tieflage (tiefe Temperaturen) bis zum duktilen Reissen in der Hochlage (hohe Temperaturen) und dem dazwischen liegenden Bereich des Steilabfalls der Zähigkeit.
Ziel des Forschungsprojektes HSK-AN-6305 war, die zentralen Elemente der neuen Richtlinie HSK-AN-425 Rev. 5 durch experimentelle Überprüfung an vergleichbaren Werkstoffen aus dem RDB Biblis C zu validieren (Einfluss der Risslänge, Fortsetzung der MC im oberen ZSÜ-Bereich). Allfällige Schwachstellen der Richtlinie HSK-AN-425 sind zu korrigieren, bevor sie in der Überwachung der Kernanlagen freigegeben werden kann. Der Einfluss der Probendicke und der Probenart auf die MC-Referenztemperatur T0 ist zu bestimmen (Übertragbarkeit der Ergebnisse auf Bauteile und Komponenten), und ob bei den Bruchmechanikproben der herkömmliche Ermüdungsanriss durch EDM-Kerben ersetzbar ist.
In dieser Publikation werden die Hauptergebnisse des Forschungsprojektes HSK-AN-6305 vorgestellt.
Keywords: fracture mechanics; quasistatic; dynamic; Master Curve; crack growth resistance curve; R curve; ASTM E 1921; ASTM E 1820; NM method; HSK-AN-425; HSK AN 425; stretch zone
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Article, self-published (no contribution to HZDR-Annual report)
Forschungszentrum Rossendorf 2009
FZD\FWS\2009\08
16 Seiten
ISSN: 1437-322X
Permalink: https://www.hzdr.de/publications/Publ-13198
Complexation of U(VI) with Nitrogen and Phosphorous Containing Ligands in Aqueous Solution
Raditzky, B.; Schmeide, K.; Sachs, S.; Bernhard, G.
Abstract
The long-term safety assessment of nuclear waste disposals requires detailed knowledge of the transport and interaction behavior of actinides within the technical, geotechnical and geological barriers. In the case of accidental release of radionuclides into the surrounding environment, their migration behavior can be effectively influenced by the ambient conditions like pH, temperature, ionic strength and especially the presence of inorganic and organic complexing ligands, e.g. bioligands like humic acids, amino acids or phospholipids. Due to their high complexing capacity towards metal ions these ligands may influence the mobility of actinides.
We studied the U(VI) complexation with nitrogen and phosphorous containing model ligands in order to simulate the functionalities of bioligands. The aim of this work is to determine the influence of various nitrogen and phosphorous containing functional groups on the U(VI) complexation and to evaluate their contribution in comparison to oxygen containing functional groups. As nitrogen containing ligands we used the biologically important substances anthranilic acid (AA) and nicotinic acid (NA). Furthermore, phenylphosphonic acid (PPA) was used as aromatic phosphorous containing ligand.
The complexation studies in aqueous solution were performed as a function of pH using time-resolved laser-induced fluorescence spectroscopy (TRLFS). All ligands show a complex formation with U(VI) under the given experimental conditions ([U(VI)] = 0.05 mM, [ligand] = 0 0.5 mM, pH 2-4, I = 0.1 M, T = 25°C). The binding of U(VI) by AA and NA takes place via the carboxylic group of the ligands. It can be concluded, that oxygen containing functional groups dominate the U(VI) complexation in the investigated pH range. The nitrogen functionalities of the ligands play only a subordinate role. AA forms a 1:1 complex, with a corresponding stability constant of log ß11 = 3.14 +/- 0.17 [1]. The formation of 1:1 and 1:2 complexes was detected for the U(VI)-nicotinate system (log ß11 = 3.73 +/- 0.30, log ß12 = 7.46 +/- 0.17 [1]) as well as for the U(VI)-phenylphosphonate system (log ß11 = 3.58 +/- 0.17, log ß12 = 6.81 +/- 0.10). At high U(VI) concentrations (1 mM), a precipitation of the formed complexes was observed for the U(VI) complexation by AA and PPA. The precipitates were analyzed with FT-IR spectroscopy and X-ray diffraction. To study the influence of different functional groups on the complexation of actinides in different oxidation states, comparable complexation studies are performed with Am(III).
References:
[1] B. Raditzky, K. Schmeide, S. Sachs, G. Geipel, G. Bernhard, Polyhedron (2009), doi:10.1016/j.poly.2009.08.010.
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Contribution to proceedings
RadChem 2010 - 16th Radiochemical Conference, 18.-23.04.2010, Marianske Lazne, Czech Republic -
Lecture (Conference)
RadChem 2010 - 16th Radiochemical Conference, 18.-23.04.2010, Marianske Lazne, Czech Republic
Permalink: https://www.hzdr.de/publications/Publ-13197
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