Publications Repository - Helmholtz-Zentrum Dresden-Rossendorf

"Online First" included
Without submitted and only approved publications
Only approved publications

31836 Publications
Proceedings of the 6th International Conference on Computer Simulation of Radiation Effects in Solids (COSIRES 2002), June 23 - 27, Dresden, Germany
Möller, W.; Posselt, M.; Jäger, H.-U.;
Proceedings volume!
Keywords: Computer simulation, Radiation Effects in Solids
  • Nuclear Instruments and Methods in Physics Research B 202 (2003)

Publ.-Id: 5379 - Permalink

Improvement of the repulsive part of the classical interatomic potential for SiC
Belko, V.; Posselt, M.; Chagarov, E.;
In order to enable a better description of ballistic and athermal processes occurring in the initial stage of ion-beam-induced defect formation, the repulsive part of the interatomic potentials of Gao and Tersoff is improved. The first modification concerns the two-body part of the potentials. At small interatomic distances it is replaced by the well-tested potential of Ziegler, Biersack, and Littmark (ZBL). For repulsive interactions between zero and some ten electron volt, an exponential spline function is employed to connect the ZBL potential with the two-body parts of the Tersoff and the Gao potential. The modified two-body potentials and their first derivatives are continuous and monotonic over the whole range of repulsive interaction. They are in good agreement with data obtained by density-functional-theory calculations. Furthermore, the three-body part of the Tersoff and the Gao potential is modified in order to avoid the strong dependence of repulsive interactions between two atoms on the bond-order parameter, i.e. on their coordinations. The modification is performed in such a manner that the total potential and its first derivative remain continuous and monotonic for all repulsive interactions.
Keywords: Interatomic Potential, SiC, Molecular Dynamics, Computer simulations
  • Nuclear Instruments and Methods in Physics Research B 202 (2003) 18-23

Publ.-Id: 5378 - Permalink

Needle shaped conductivity probes with integrated micro-thermocouple and their application in rapid condensation experiments with non-condensable gases
Prasser, H.-M.; Böttger, A.; Zschau, J.; Gocht, T.;
The present paper deals with advanced conductivity probes for local void measurements, which were equipped with a micro-thermocouple, which is integrated into the probe at the place of the electrode wire. These probes were used for rapid transient condensation tests in a heat exchanger pipe immersed into a cooling water tank. The experiments serve as data sources for the validation of thermal-hydraulic system codes concerning the modelling of the condensation, particularly with respect to the behaviour and effect of non-condensable gases. The present tests were carried out at the pressurizer test facility DHVA of the University for Applied Sciences in Zittau/Görlitz serving as steam source. The slightly downwards inclined condensation tube was connected to the head of the pressure vessel and supplied with steam in this way. The application of a new type of two-phase instrumentation has revealed details about the transient condensation process. Since test were performed with and without the presence of a non-condensable gas (air), the effect of the gas could be studied. The merits of the probes lie in the ability to distinguish between steam and gas. Without the synchronous temperature and void measurement performed by the probes it would have not been possible to clarify the physical background of the temperature jumps found during the experiments with the non-condensable gas.

Keywords: steam condensation, non-condensable gas, local void probes, micro-thermocouples, transients
  • Kerntechnik 68 (2003) 3, pp. 114-120.

Publ.-Id: 5377 - Permalink

Innovative transient-proof hydrostatic level measuring method
Gocht, T.; Traichel, A.; Hampel, R.; Prasser, H.-M.;
Most of the level monitoring systems for pressure vessels containing saturated steam-water mixture use the hydrostatic method. Differential pressure transducers are connected by pulse tubes with nozzles at different height of the pressure vessel. A disadvantage of this method is given by measuring errors cause by evaporation and/or degassing processes in vertical parts of these pulse lines. The error is caused by the decrease of the fluid density in the reference pipe, when a two-phase mixture appears. The present work aimed at the test of a novel differential pressure measuring system that eliminates the influence of density changes in the pulse lines. It is based on two differential pressure transducers, placed accurately at the elevation of the connecting nozzles. They are connected with the pressure vessel only by horizontal pipes. The vertical distance is bridged by a standpipe, the fluid of which is completely separated from the fluid in the vessel. Degassing respectively evaporation effects can therefore completely excluded in the reference column of the new system. The method was tested at the pressurizer test facility of the University of Applied Sciences Zittau/Görlitz on three types of transients including a rapid pressure decrease similar to a loss-of-coolant transient. Traditional differential pressure systems as well as local void probes were used for comparison. The method has proven its advantages compared to the traditional hydrostatic level measurement method.
Keywords: hydrostatic level measurement, differential pressure transducer, local void probes
  • Kerntechnik 68 (2003) 3, pp. 97-101.

Publ.-Id: 5376 - Permalink

Untersuchungen zur strukturellen Modellverbesserung durch Symbiosen zwischen Modellen
Hoppe, D.;
Im Zuge von Modellbildungen ist es nicht immer möglich, das zu beschreibende Objekt sofort oder direkt durch ein einzelnes Modell vollständig zu erfassen. Vielmehr wird es zunächst mehrere untergeordnete Modelle geben, die jeweils nur verschiedene eingeschränkte Sichten auf das Objekt repräsentieren. Im Beitrag wird untersucht, wie solche Modelle zu einer Modellsymbiose verbunden werden können und wie mit deren Hilfe dann nach einem verbesserten Einzelmodell des zu beschreibenden Objektes gesucht werden kann.
  • Open Access LogoWissenschaftlich-Technische Berichte / Forschungszentrum Rossendorf; FZR-374 April 2003


Publ.-Id: 5375 - Permalink

Organic chemistry with the short-lived positron emitters 11C and 18F
Wüst, F. R.;
Positron emission tomography (PET) is a powerful imaging technique for the in vivo study of molecular interactions and molecular pathways in the human body. In combination with approprately labelled radiotracers, PET offers exceptional possibilities to study physiology, metabolism, pharmacokinetics and modes of action of novel and established drugs, and food ingredients.

The key element of PET is the PET-radiotracer, a compound labelled with a short-lived positron emitter. The most useful positron emitters for the labelling of organic moleculars are 11C and 18F which have half-lives measured in minutes, bein 20.4 min and 109.6 min, respectively. Consequently, time dominates all aspects of PET. In this connection the extensive performance of organic radiochemistry using 11C and 18F is fundamental but also a special challenge. This review will address the recent developemts of organic PET radiochemistry in the synthesis of PET radiotracers with special focus on 11C and 18F
Keywords: positron emission tomography, organic PET chemistry, radiolabelling techniques
  • Trends in Organic Chemistry (2003) 10: 61-70

Publ.-Id: 5374 - Permalink

A new Cryptophane Receptor Featuring Three endo-Carboxylic Acid Groups: Synthesis, Host Behavior and Structural Study
Roesky, C. E. O.; Weber, E.; Rambusch, T.; Stephan, H.; Gloe, K.; Czugler, M.;
Examples of a new type of cryptophane molecule incorporating aromatic groups in the bridges (1 - 4) and for the first time, being also supplied with three endo-positional ionizable carboxylic acid function (1) have been synthesized and characterized. The cryptophane triester 2 yielded a solvate (channel inclusion compound) with trichloromethane and water, the X-ray crystal structure of which is reported. The complexation of 1 with low-molecular-weight alcohols in solution was studied, and the liquid-liquid extraction of different metal ions including alkali (Na+, Cs+), alkaline earth (Mg2+, Ca2+, Sr2+, Ba2+), and the lanthanide metal ions Eu3+ and Yb3+ in an extraction system containing metal nitrate buffer/H2O/1/CHCl3 was examined. Molecular modeling calculations of the cryptophanes 1 and 2, and of the Eu3+ complex of 1 were carried out contributing to the discussion.
Keywords: cryptophanes, molecular modeling, molecular recognition, solvent extraction, structure elucidation
  • Chemistry, A European Journal 9/5 (2003) 1104-1112

Publ.-Id: 5373 - Permalink

Infrared Characterization of Environmental Samples by Pulsed Photothermal Spectroscopy
Seidel, W.; Foerstendorf, H.; Heise, K. H.; Nicolai, R.; Schamlott, A.; Ortega, J. M.; Glotin, F.; Prazeres, R.;
Low concentration of toxic radioactive metals in environmental samples often limits the interpretation of results of infrared studies investigating the interaction processes between the metal ions and environmental compartments. For the first time, we show that photothermal infrared spectroscopy performed with a pulsed free electron laser can provide reliable infrared spectra throughout a distinct spectral range of interest. In this model investigation, we provide vibrational absorption spectra of a rare earth metal salt dissolved in a KBr matrix and a natural calcite sample obtained by thermal beam deflection technique and FT-IR spectroscopy, respectively. General agreement was found between all spectra of the different recording techniques. Spectral deviations were observed with samples containing low concentration of the rare earth metal salt indicating a lower detection limit of the photothermal method compared to conventional FT-IR spectroscopy.

Publ.-Id: 5372 - Permalink

Brazing of alumina ceramics modified by pulsed plasma beams combined with arc PVD treatment
Piekoszewski, J.; Krajewski, A.; Prokert, F.; Senkara, J.; Stanislawski, J.; Walis, L.; Werner, Z.; Wlosinski, W.;
A new method of preparing alumina ceramic surface for brazing it to kovar with conventional Ag-Cu eutectic brazes is presented. The key concept of this approach consists in formation of two inter-layers on the ceramic surface: (i) thin (in nm scale) layer of TiOx using pulse plasma beams, and (ii) thicker (about 2 µm) layer of TiOx or metallic Ti using arc PVD technique. Grazing incidence X-ray diffraction (GXRD) analysis shows that the first layer consists most likely of Ti7O13, whereas the second is either Ti2O, or metallic Ti - depending on the deposition conditions. Commercial housings of semiconductor diodes have been used as the samples. Brazed housings were tested under routine industrial conditions. The ultimate tensile strength (UTS) of joints reaches the average value of 90 MPa. Vacuum tightness is better than 5x10-6 mbar l/s. The values of parameters are sufficient to pass the production requirements.
Keywords: Brazing of alumina; Pulsed plasma treatment
  • Vacuum 70 (2003) 307-312

Publ.-Id: 5371 - Permalink

Schmelzerückhaltung im RDB nach Verlagerung von Corium in das untere Plenum Zusammenfassung der bisherigen Ergebnisse des Projekts Nr.: 150 1254
Altstadt, E.; Willschütz, H.-G.;
Bezüglich eines hypothetischen Kernschmelzeszenarios in einem Leichtwasserreaktor ist es notwendig, mögliche Versagensformen des Reaktordruckbehälters sowie Versagenszeiträume zu untersuchen, um die Belastung für das Containment bestimmen zu können. Es wurden bereits eine Reihe von Experimenten durchgeführt, welche Erkenntnisse hierüber liefern sollen. Begleitend wurden in Einzelversuchen Materialeigenschaften ermittelt, sowie theoretische und numerische Arbeiten durchgeführt.
Für die Simulation von Experimenten zum Versagen der Bodenkalotte, wie OLHF oder FOREVER, ist es notwendig, Kriechen und Plastizität zu berücksichtigen. Gleichzeitig müssen geeignete Modelle das Temperaturfeld in der Behälterwand für die mechanischen Rechnungen bereitstellen. Vom Institut für Sicherheitsforschung des FZR wird ein Finite-Elemente-Modell erstellt, das sowohl die Temperaturfeldberechnung für die Wand als auch die elasto-plastische Mechanik der Behälterwand modelliert. Die bisher durchgeführten Arbeiten werden in diesem Bericht kurz erläutert und mit Beispielen belegt.
Am FZR wurde ein Finite-Elemente-Model entwickelt, das die Verwendung von einfachen Kriechgesetzen, die mit ihren angepassten Konstanten nur für begrenzte Spannungs- und Temperaturbereiche gültig sind, umgeht. Stattdessen wird eine numerische Kriechdatenbasis angelegt, in der die Kriechdehnrate in Abhängigkeit von der Gesamtdehnung, der Temperatur und der Vergleichsspannung abgelegt ist. Eine wesentliche Aufgabe für diese Vorgehensweise besteht in der Generierung und Validierung der Kriechdatenbasis. Zusätzlich wurden alle relevanten temperaturabhängigen Materialeigenschaften mit entsprechenden Modellen in den Code eingegeben. Für die Bestimmung der Versagenszeit wurde ein Schädigungsmodel nach einem Vorschlag von Lemaitre implementiert.
Die Validierung des numerischen Models erfolgt durch die Simulation von und den Vergleich mit Experimenten. Dies geschieht in 3 Stufen: zunächst werden einzelne einachsige Kriechversuche nachgerechnet, was als 1D-Problem bezeichnet wird. In der nächsten Stufe werden sogenannte ¿Rohrversagensexperimente¿ simuliert: das RUPTHER-14 und das ¿MPA-Meppen¿-Experiment. Diese Experimnete werden als 2D-Probleme betrachtet. Schließlich kann das Modell auf skalierte 3D-Versuche angewendet werden, in denen die Bodenkalotte eines Druckwasserreaktors mit ihrer halbkugelförmigen Geometrie wiedergegeben wird. Ein Beispiel hierfür sind die FOREVER-Experimente. In Zusammenarbeit mit den Experimentatoren an der KTH in Stockholm wurden Pre- und Posttest-Rechnungen für diese bisher einzigartigen Experimente durchgeführt, deren Ergebnisse qualitativ und quantitativ sehr zufriedenstellend sind.
Eine wichtige Frage im Rahmen dieser Arbeit ist die Vergleichbarkeit des französischen Reaktordruckbehälterstahls 16MND5 und des deutschen 20MnMoNi5-5, welche chemisch nahezu identisch sind. Da diese beiden Stähle ein ähnliches Verhalten zeigen, sollte es in gewissem Umfang zulässig sein, experimentelle und numerische Daten und Erkenntnisse zwischen beiden zu übertragen.
Keywords: Kernschmelzszenario im Leichtwasserreaktor, Kriechvorgang der Druckbehälterwand, Finite Elemente Simulation, Entwicklung einer Materialdatenbank
  • Open Access LogoWissenschaftlich-Technische Berichte / Forschungszentrum Rossendorf; FZR-370 März 2003


Publ.-Id: 5370 - Permalink

On the temperature dependence of the electric characteristics and mass spectra of liquid metal alloy ion sources
Ganetsos, T.; Mair, G. L. R.; Bischoff, L.;
This paper reports on an extensive study of the characteristics of AuGeSi and CoNd liquid metal alloy ion sources (Focused Ion Beams From Liquid Metal Ion Sources,Research Studies Press,Taunton,Somerset,UK,1991).Such characteristics include current –voltage curves and ion beam mass spectra.A careful investigation has been undertaken where the emitter temperature is the main variable experimental parameter.Theoretical models,or theoretical attempts in certain cases,tend to support the experimental results.The experimental results,in conjunction with existing theories, suggest that simply for reasons of self-consistency two mechanisms must be operative for the production of doubly- charged ions from the AuGeSi source:direct .eld-evaporation and post-ionisation.
Keywords: Surface tension:Implantation:Microelectronics
  • Ultramicroscopy 95 (2003) 171 - 181

Publ.-Id: 5369 - Permalink

Do Perchlorate and Triflate Anions Bind to the Uranyl Cation in an Acidic Aqueous Medium? A Combined EXAFS and Quantum Mechanical Investigation
Sémon, L.; Boehme, C.; Billard, I.; Hennig, C.; Lützenkirchen, K.; Roßberg, A.; Rossini, I.; Wipff, G.;
  • Chemphyschem 2001, 2, 591-598

Publ.-Id: 5367 - Permalink

Surface plasmon transmission across narrow grooves in thin silver films
Seidel, J.; Grafström, S.; Eng, L.; Bischoff, L.;
We report on the direct measurement of surface plasmon transmissivity of narrow grooves in thin silver films using near-field optical microscopy in an attenuated-total-reflection setup. For different groove widths, we observe characteristic changes in transmissivity that are attributed to resonant gap modes. The results are in good agreement with existing theoretical predictions.
Keywords: Surface plasmon, narrow groves, focused ion beam, silver films

Publ.-Id: 5366 - Permalink

Energiedispersive Untersuchung der Wechselwirkung schneller Neutronen mit Materie; Teilbericht : Auslegung des Neutronen-Produktionstargets
Altstadt, E.; Beckert, C.; Eckert, S.; Freiesleben, H.; Galindo, V.; Grosse, E.; Naumann, B.; Weiß, F.-P.;
Der Aufbau und die erste Nutzung eines kompakten Flugzeitsystems zur energiedispersiven Untersuchung der Wechselwirkung von schnellen Neutronen mit Materialien sind Inhalt eines Vernetzungsprojektes des Forschungszentrums Rossendorf, an dem auch die Technische Universität Dresden im Rahmen eines gemeinsamen DFG-Projektes mitarbeitet. Die geplanten Flugzeit-Experimente mit gepulsten Neutronen werden an der Strahlungsquelle ELBE durchgeführt werden. Erste Ergebnisse zur Entwicklung eines Neutronen-Produktionstargets werden vorgestellt. Mit Hilfe von Strahlungstransport- und Finite-Elemente-Programmen wurden die Verteilungen der Energiefreisetzung des von der Strahlungsquelle ELBE genutzten Elektronenstrahls und der Temperatur im Neutronen-Radiator sowie die zu erwartenden Teilchenspektren und -flüsse am Messplatz berechnet. Überlegungen zur Entwicklung des Strahlfängers werden diskutiert.
Keywords: Photoneutronen, Neutronenfluss, Flugzeit-Experimente, Strahlungsquelle ELBE, Neutronen-Radiator, Dosisleistung, Abschirmung, Strahlf"anger
  • Open Access LogoWissenschaftlich-Technische Berichte / Forschungszentrum Rossendorf; FZR-369 März 2003


Publ.-Id: 5365 - Permalink

The mineral-specific thermodynamic sorption database RES3T: Concept description, implementation, and application towards contaminated systems
Richter, A.; Brendler, V.; Bernhard, G.;
RES3T – the Rossendorf Expert System for Surface and Sorption Thermodynamics – is a digitized thermodynamic sorption database utilizing surface complexation models (SCM). It is mineral-specific and can therefore also be used for complex models of solid phases such as rocks or soils. As to the knowledge of the authors there is no such digital thermodynamic database for surface complexation equilibria existent worldwide, despite of the vast amount of available data.
Data records comprise of mineral properties, specific surface area values,characteristics of surface binding sites and their protolysis, sorption ligand information, and surface complexation reactions. An extensive bibliography is also included, providing links not only to the above listed data items, but also to background information concerning surface complexation model theories, surface species evidence, and sorption experiment techniques.
An integrated user interface helps users to access selected mineral and sorption data, to extract internally consistent data sets for sorption modeling, and to export them into formats suitable for other modeling software. It assists the identification of critical data gaps, the evaluation of existing parameter sets, consistency tests and the establishing of selected reference data sets.
RES3T is implemented as a relational database under MS ACCESS. The database is intended for an international use and is currently converted into a WWW-based version.
A system for illustrating the current blind predictive capabilities of SCM using the RES3T database is the Cu2+ sorption onto iron oxyhydroxides. To keep the number of parameters at a minimum, the Diffuse Double Layer model was selected to account for electrostatics. The calculation was performed with the FITEQL code, version 3.2. The respective SCM parameters from RES³T were the binding site density for the minerals, the surface protolysis constants, and the brutto stability constants for all relevant surface complexes. The model prediction almost always represented the experimental values for the sorbed amount of Cu2+, expressed as conventional distribution coefficients KD as required by PA software.

Keywords: sorption, database, RES3T,SCM, surface complexation model, Access, diffuse double layer
  • Lecture (Conference)
    Goldschmidt Conference 2003, 7.-12.9.03, Kurashiki, Japan
  • Abstract in refereed journal
    Geochimica et Cosmochimica Acta 67 (2003): A397

Publ.-Id: 5364 - Permalink

Structure determination by combined X-ray diffraction and X-ray absorption spectroscopy measurements using synchrotron radiation
Hennig, C.;
  • Lecture (Conference)
    ANKA FSG Seminar, Karlsruhe, Germany, 14.01.2002

Publ.-Id: 5362 - Permalink

XAFS-Untersuchungen von Actinidensystemen mittels Synchrotronstrahlung
Hennig, C.;
  • Lecture (Conference)
    XAFS-/NANES-Symposium, Rossendorf, Germany, 12.04.2002

Publ.-Id: 5361 - Permalink

Structure of uranium(VI) complexes sorbed at 1:1 and 2:1 clay mineral surfaces - A comparative ESAFS study
Hennig, C.;
  • Lecture (Conference)
    Mineral Surface and Colloid Chemistry in Soil and Aquatic Environments, Karlsruhe, Germany, 08.-09.10.2002

Publ.-Id: 5359 - Permalink

Application of X-ray absorption spectroscopy to determine uptake processes of uranium at the clay mineral surface
Hennig, C.;
  • Lecture (Conference)
    Polytechnical University of Catalonia, Barcelona, Spain, 18. 10. 2002

Publ.-Id: 5358 - Permalink

investigation of Actinide complex compounds with X-ray absorption spectroscopy
Hennig, C.;
  • Lecture (Conference)
    ESRF SAC Meeting, Grenoble, France, 08.11.2002

Publ.-Id: 5357 - Permalink

Untersuchungen zur Mineralauflösung von unterschiedlich alterierten Chloriten und deren Einfluss auf die Sorption von U(VI)
Krawczyk-Bärsch, E.; Arnold, T.; Brandt, F.; Bosbach, D.; Bernhard, G.;
Mit Batch- und Durchflussexperimenten wurde, unter Einbeziehung der Mineralauflösung und Sekundärphasenbildung, die U(VI) Sorption auf zwei unterschiedlichen Chloritmineralen untersucht. Hierbei handelte es sich um einen nicht alterierten Ripidolith Chlorit (CCa-2) von Flagstaff Hill (El Dorado County, California, USA), der aus einem Chloritschiefer gewonnen wurde und einen hydrothermal alterierten Chlorit von Grimsel (Schweiz), der aus einer granitischen Kluft gewonnen wurde. Die Durchflussexperimente wurden mit 0,5 g des jeweiligen Chloritpulvers (63-200 µm Korngröße), einer 0.1 M NaClO4-Ausgangslösung, einer U(VI)-Konzentration von 1´10-6 M und bei einem pH von 6,5 durchgeführt. Die Ergebnisse zeigten einen deutlichen Unterschied im Sorptionsverhalten der beiden Chlorite. Der nicht alterierte CCa-2 Chlorit zeigte ein Sorptionsmaximum von 90 % und wies damit eine mehr als 20 % höhere Sorption unter vergleichbaren Bedingungen als der hydrothermal alterierte Chlorit auf. Vorangegangene Untersuchungen am CCa-2 Chlorit [1] und Grimsel Chlorit [2] zeigten, dass diese erhöhte Sorption auf die Bildung von Fe-oxyhydroxiden, wie beispielsweise Ferrihydrit, während der Auflösung des nicht alterierten Chlorits zurückgeführt werden können. Ferrihydrit ist aufgrund seiner hohen spezifischen Oberfläche und seiner hohen Sorptionsaffinität ein wichtiger Sorbent für U(VI). Der alterierte Grimsel Chlorit wurde bereits im hydrothermalen Stadium gelaugt, so dass dieser nicht so stark zur Sekundärphasenbildung neigt wie der CCa-2 Chlorit. Die unterschiedlichen U(VI) Sorptionsergebnisse an den beiden Chloriten belegen diese Interpretation.
/1/ Krawczyk-Bärsch et al. (2003): Chem. Geol. (submitted).
/2/ Arnold et al., (1998): Chem. Geol. 151, 129-141.
  • Lecture (Conference)
    GDCH-Hauptversammlung München 6.-11.10.2003

Publ.-Id: 5356 - Permalink

Modellbasiertes Online-Zustandserkennungssystem für exotherme chemische Prozesse
Hessel, G.; Kryk, H.; Schmitt, W.; Seiler, T.; Weiß, F.-P.; Hilpert, R.; Roth, M.;
Bei stark exothermen Batch- und Semibatch-Prozessen ist die Identifikation des aktuellen Prozesszustandes und die frühzeitige Erkennung von unerwünschten Betriebszuständen sowohl unter dem Aspekt der Anlagen- und Umweltsicherheit als auch aus Gründen der Sicherung einer gleichbleibend hohen Ausbeute und Produktqualität von besonderer Bedeutung. Zur Unterstützung des Bedienungspersonals hinsichtlich einer optimalen Anlagenfahrweise wurde ein auf adaptiven Energie- und Stoffbilanzen basierendes Online-Monitoring-System (MoSys) konzipiert. Die Systementwicklung erfolgte anwendungsorientiert für heterogen katalysierte Hydrierprozesse von Nitroaromaten in Rührkesselreaktoren. Für den Einsatz des Systems im Industriemaßstab wurde MoSys in ein komplexes Batch-Informations-Management-System (BIMS) eingebunden. Somit ist die Anzeige der MoSys-Ergebnisse, wie Umsatz- und Konzentrationsverläufe, simultan zu den primären Prozesssignalen und den chargenorientierten Informationen an den verschiedenen Operatorstationen in der Chemieanlage möglich. Der Test des Zustandserkennungssystems erfolgte an einer Mehrzweckanlage der DEGUSSA AG im Werk Radebeul.
Gezeigt werden der prinzipielle Aufbau des Monitoring-Systems (Berechnungsalgorithmus), die Einbindung und Funktion von MoSys innerhalb des Batch-Informations-Management-Systems sowie die Visualisierung der MoSys-Ergebnisse an den Operatorstationen am Beispiel von einzelnen Screenshots. Die Validierung des Systems an der Industrieanlage ist am Beispiel von Konzentrations- und Umsatzverläufen sowie der Zustandsklassifikation für die Zwischenproduktakkumulation dargestellt. Eine Zusammenfassung, in der die Bedeutung des Einsatzes von BIMS/MoSys für die industrielle Praxis aufgezeigt wird, beschließt den Artikel.
  • Technische Überwachung Bd. 44, Nr. 5 (2003) 43-47

Publ.-Id: 5355 - Permalink

Nachweis adsorbierter U(VI) Oberflächenspezies auf Muskovit mit TRLFS
Arnold, T.; Geipel, G.; Brendler, V.; Bernhard, G.;
Mittels zeitaufgelöster laserinduzierter Fluoreszenzspektroskopie (TRLFS) wurde die Uranyl(VI) Sorption auf dem Schichtsilikatmineral Muskovit angewendet. Ziel dabei war es, die adsorbierten Oberflächenspezies sowohl auf den Basisflächen als auch auf den Kantenflächen nachzuweisen und zu vergleichen.
Die Muskovit Plättchen wurden dazu bei pH 6.3 für ca. 60 h mit einer 1×10-5 M Uranyl Lösung (0,1 N NaClO4) kontaktiert. Etwa 72 % der Ausgangsmenge an Uranyl wurde unter diesen Bedingungen sorbiert.
Auf den Basisflächen wurde kein Uranyl-Fluoreszenzspektrum erhalten, was zeigt, dass Uranyl vernachlässigbar sorbiert wurde (< 10-12 M/cm2). Die Sorption erfolgt dominierend an den Kantenflächen. Die Spektrenauswertung ergab das Vorliegen von zwei sorbierten Uranylspezies mit Lebensdauern von 1,15 bzw. 9,65 µs. Die Lage der Hauptemissionsbanden stimmen innerhalb der Fehlergrenzen für beide Komplexe überein, was auf eine unterschiedliche Anzahl der umgebenden Wassermoleküle hinweist. Aus diesen Ergebnissen und zusätzlich durchgeführten EXAFS Untersuchungen lässt sich die Sorption von Uranyl(VI) an den Muskovit Kantenflächen am besten mit zwei bidentaten mononuklearen Oberflächenspezies beschreiben.
  • Lecture (Conference)
    GDCH-Hauptversammlung München 6.-11.10.2003

Publ.-Id: 5354 - Permalink

An X-ray absorption spectroscopy study of neptunium(V) reactions with mackinawite (FeS)
Moyes, L. N.; Jones, M. J.; Reed, W. A.; Livens, F. R.; Charnock, J. M.; Mosselmans, J. F. W.; Hennig, C.; Vaughan, D. J.; Pattrick, R. A. D.;
  • Environ. Sci. Technol. 36 (2002) 179 - 183

Publ.-Id: 5352 - Permalink

Synchrotron Radiation for Study of Radioactive Materials
Hennig, C.;
  • Other report
    Digest Report of the XIV Russian Synchrotron Radiation Conference, Novosibirsk, Russia, 15.-19.07.2002

Publ.-Id: 5351 - Permalink

EXAFS and XRD investigations of zeunerite and meta-zeunerite
Hennig, C.; Reck, G.; Reich, T.; Rpoßberg, A.; Kraus, W.; Sieler, J.;
  • Zeitsschrift für Kristallographie, 21 (2003) 37-45

Publ.-Id: 5350 - Permalink

Alloy liquid metal ion sources for mass separated focused ion beams
Bischoff, L.; Mair, G. L. R.;
During the last decades, the focused ion beam (FIB) became a very useful and versatile tool in the microelectronics industry, as well as in the field of research and development. For special purposes like writing ion implantation or ion mixing in the µm- or sub-µm range different ion species are needed. Therefore alloy liquid metal ion sources (LMIS) are used. The energy distribution of the ions from an alloy LMIS is one of the determining factors for the performance of an FIB column. Different source materials like Au73Ge27, Au82Si18, Au77Ge14Si9, Co36Nd64, Er69Ni31, and Er70Fe22Ni5Cr3 were investigated with respect to the energy spread of the different ion species as a function of emission current I, ion mass m and emitter temperature T. For singly charged ions the predicted dependence of the energy spread, DE µ I2/3 m1/3 T1/2 found for Ga could be confirmed. The alloy LMIS`s discussed above have been used in the Rossendorf FIB system IMSA-100 especially for writing implantation to fabricate sub-µm pattern without any lithographic steps. A Co-FIB was applied for the ion beam synthesis of CoSi2 micro-structures. Additionally, the possibility of varying the current density with the FIB by changing the pixel dwell-time was used for radiation damage investigations in Si and SiC at elevated implantation temperatures. Furthermore, a broad spectrum of ions was employed to study the sputtering process depending on temperature, angle of incidence and ion mass on a couple of target materials using the volume loss method. Especially this technique was used for the fabrication of various kinds of micro-tools.
All these examples underline the importance of FIBs in modern research and the new possibilities opened up by a mass separated system applying a broad spectrum of ion species.

Keywords: alloy liquid metal ion source, mass-separated focused ion beam, applications
  • Recent Research Developments in APPLIED PHYSICS, 6 (2003) 123 - 133 Transworld Research Network, Trivandrum, India ISBN: 81-7895-085-5

Publ.-Id: 5348 - Permalink

Control of floating-zone single crystal growth by magnetic fields
Hermann, R.; Behr, G.; Gerbeth, G.; Priede, J.; Schultz, L.;
The aim of the investigation is the growth of high-precision single crystals of intermetallic compounds using well defined magnetic fields. The fundamental problem is conditional on the fact that especially complicated intermetallic compounds are not producible as single crystals over the whole cross-section by the inductive floating-zone melting technique since the geometry of the zone at the solid-liquid-interface is unfavourable. The controlled adjustment of a solid-liquid-interface of desired curvature and the knowledge of the melt convection in liquids with high conductivity can be arranged by the contact-less influence of electromagnetic fields. Numerical simulations for the determination of the electromagnetic field configuration induced by the RF heater coil and the solution of the coupled heat and hydrodynamic equations were done for the model substance Ni [1]. The significant influence of the electromagnetically driven flow, which acts opposite to the Marangoni convection, makes the solid-liquid interface concave towards the melt.
Comprehensive investigations of the influence of growth parameters such as zone length, power influence and heated region on the solid-liquid interface geometry during RF floating zone crystal growth were carried out experimentally. It could be shown that undesired concave (towards the melt) interface regions cannot be avoided even at optimised parameter configurations [2].
As a result, a two-phase magnetic field pump, which allows a strong manipulation of the convection and therefore of the solid-liquid interface, was designed. It allows to change the flow structure from the typical double vortex to a single one with a strong influence on the phase boundary shape (Fig. 1). The adjustment of a complete convex solid-liquid interface shape in RF-floating zone crystal growth was tackled with this additional melt stirring resulting in a definite improvement of the solid-liquid-interface.
  • Poster
    2nd French German Crystal Growth Meeting, 10th-13th March 2003, Nancy, FRANCE

Publ.-Id: 5347 - Permalink

Uranium(VI) Complexation by Calix[6]arenes studied by Time-resolved Laser-induced Fluorescence Spectroscopy (TRLFS)
Schmeide, K.; Geipel, G.; Ludwig, R.; Heise, K. H.; Bernhard, G.;
For the purification of uranium contaminated waters various water purification methods (e.g., application of ion exchangers, direct precipitation, microbiological methods) are usually applied. Also solvent extraction applying calix[6]arenes is suitable to separate uranium from aqueous solution [1]. To facilitate the uranium separation from uranium containing waters in practice, we are developing an alternative procedure. For this, calix[6]arenes are permanently fixed onto textile substrates via spacer groups [2]. This method is advantageous especially for smaller remediation objects and objects with lower contamination levels ([UO22+] ~ 1×10-6 M).
In the present work, the extraction efficiency of various calix[6]arenes including their selectivity towards uranium(VI) is studied in a two phases solvent extraction system in dependence on pH value, ligand concentration and the amount of competing ions. The complex formation between uranium(VI) and calix[6]arenes is further studied at pH 4 by means of TRLFS as well as by TRLFS with ultrashort laser pulses. By these methods it is possible to detect uranium and calixarene species at equilibrium directly in the aqueous and organic phase. Reaction mechanisms are discussed and extraction constants are determined. In the presence of competing ions (e.g., calcium, barium, magnesium) the uranium extraction is only slightly decreased. The suitability of the calix[6]arenes as efficient reagents for selective uranium separation from aqueous solution is shown.

[1] Shinkai, S. et al.: Molecular design of calixarene-based uranophiles which exhibit remarkably high stability and selectivity. J. Am. Chem. Soc. 109, 6371-6376 (1987).
[2] Schmeide, K. et al.: Separation of uranium from aqueous solution by textile bound calixarenes. In: Uranium in the aquatic environment. Springer Verlag, Berlin 2002, p. 417-424.
Keywords: Uranium, Calixarene, Complexation, TRLFS
  • Poster
    9th International Conference on Chemistry and Migration Behavior of Actinides and Fission Products in the Geosphere: Migration'03, Gyeongju, Korea, 21.-26.09.2003

Publ.-Id: 5345 - Permalink

Washout studies of 11C in rabbit thigh muscle implanted by secondary beams of HIMAC.
Tomitani, T.; Pawelke, J.; Kanazawa, M.; Yoshikawa, K.; Yoshida, K.; Sato, M.; Takami, T.; Koga, M.; Futami, Y.; Kitagawa, A.; Urakabe, E.; Suda, M.; Mizuno, H.; Kanai, T.; Matsuura, H.; Shinoda, I.; Takizawa, S.;
Heavy ion therapy has two definite advantages: good dose localization and higher biological effect. Range calculation of the heavy ions is an important factor in treatment planning. X-ray CT numbers are used to estimate the heavy ion range by looking up values in a conversion table which relates empirically photon attenuation in tissues to particle stopping power; this is one source of uncertainty in the treatment planning. Use of positron emitting radioactive beams along with a positron emission tomograph or a positron camera gives range information and may be used as a means of checking in heavy ion treatment planning. However, the metabolism of the implanted positron emitters in a living object is unpredictable because the chemical forms of these emitters are unknown and the metabolism is dependent on the organ species and may be influenced by many factors such as blood flow rate and fluid components present. In this paper, the washout rate of 11C activity implanted by injecting energetic 11C beams into thigh muscle of a rear leg of a rabbit is presented. The washout was found to consist of two components, the shorter one was about 4.2+-1.1 min and the longer one ranged from 91 to 124 min. About one third of the implanted positron activity can be used for imaging and the rest was washed out of the target area.
  • Physics in Medicine and Biology 48 (2003) 875-889

Publ.-Id: 5344 - Permalink

Induction of micronuclei in human fibroblasts and keratinocytes by 25 kV x-rays
Slonina, D.; Spekl, K.; Panteleeva, A.; Brankovic, K.; Hoinkis, C.; Dörr, W.;
A relative biological effectiveness (RBE) not much larger than unity is usually assumed for soft x-rays (up to ~50 keV) that are applied in diagnostic radiology such as mammography, in conventional radiotherapy and in novel radiotherapy approaches such as x-ray phototherapy. On the other hand, there have been recent claims of an RBE of more than 3 for mammography and respective conventional x-rays. Detailed data on the RBE of soft x-rays, however, are scarce. The aim of the present study was to determine the effect of low-energy x-rays on chromosomal damage in vitro, interms of micronucleus induction. Experiments were performed with 25 kV x-rays and a 200 kV x-ray reference source. The studies were carried out on primary human epidermal keratinocytes (HEKn), human fibroblasts (HFIB) and NIH/3T3 mouse fibroblasts. Micronucleus (MN) induction was assayed after in vitro irradiation with doses ranging from 1 to 5.2 Gy. Compared to the effect of 200 kV x-rays, 25 kV x-rays resulted in moderately increased chromosomal damage in all cell lines studied. This increase was observed for the percentage of binucleated (BN) cells with micronuclei as well as for the number of micronuclei per BN cell.
Moreover, the increased number of micronuclei per micronucleated BN cell in human keratinocytes and 3T3 mouse fibroblasts suggests that soft x-rays induce a different quality of damage. For all cell lines studied the analysis of micronucleus induction by 25 kV soft x-rays compared to 200 kV x-rays resulted in an RBE value of about 1.3. This indicates a somewhat enhanced potential of soft x-rays for induction of genetic effects.
Keywords: soft x-rays, MN assay, human cells, RBE
  • Radiation and Environmental Biophysics 42 (2003) 55-61

Publ.-Id: 5343 - Permalink

Complex formation of uranium with 2,5-dihydroxybenzoic Acid
Geipel, G.; Nagasaki, S.; Bernhard, G.;
To study of the complex formation of dihydroxybenzoic acids with uranium(VI), we measured the spectra of 2,5-dihydroxybenzoic acid (2,5-DHBA) as a function of pH (2.0 - 4.0) and concentration of uranium (0 - 5x10-3 M). The intensity of the spectra changes with pH and uranium concentration. As we found only spectra with one emission maximum and mono-exponential fluorescence decay, we concluded that no excited state reactions could be observed in the experimental conditions. On the other hand, a change in the fluorescence lifetime could be obtained. The fluorescence lifetimes were found to be in the range from 1.8 ns to 5.7 ns. This means that a dynamic quench process occurred. In order to estimate the formation constant of the 2,5-DHBA with uranium, firstly, we evaluated the protonation constant of the carboxylic group of the 2,5-DHBA. It was found to be log K3 = 2.77 ± 0.05, by taking into account the self-quenching effect. This is in good agreement with literature data (2.82) /1/. The 2,5-DHBA itself and uranium quench the fluorescence of the 2,5-DHBA. We evaluated the dynamic quench constants to be KSV = 216 ± 4 for the ligand itself and KSV = 45 ± 1 for uranium. Both have to be taken into consideration for estimating the complex formation constant. Furthermore, in the pH range 2.0 to 4.0, slopes between 0.91 and 1.39 were found for the validation of the stoichiometry. We conclude, therefore, that a one to one complex forms between uranium and 2,5-DHBA. The dependence of the formation constants on pH values was investigated in order to determine the number of protons involved in the complex formation. Since the slope of the pH dependence was -0.79 ± 0.1, we conclude that one proton at most is involved in this complex formation. This suggests that only the carboxylic group is involved in the complex formation. Based on these considerations, the complex formation constant was assigned to be log K = -0.57 ± 0.26. As uranium shows fluorescence properties, the complex formation can be also confirmed using the changes in the fluorescence behavior of uranium. The formed complex itself does not show fluorescence properties, and only the emission of the non-complexed uranium is observed. As example at pH 4.0, formation constants of log K = 3.29 ± 0.16 were assigned for the ligand study and of log K = 3.17 ± 0.32 for the uranium study, respectively./1/ L. Lajunen, R. Portanova, J. Piispanen et al; Pure & Appl.Chem.,69,329 (1997)
  • Lecture (Conference)
    Migration 2003, Sept. Korea
  • Contribution to proceedings
    Abstract in Proceedings, 21.-26.09.2003, Gyeongiu, Korea

Publ.-Id: 5342 - Permalink

Excited state reactions in studies of complex formation between actinides and organic ligands with laser induced methods
Geipel, G.; Bernhard, G.; Vulpius, D.;
In a former study we analyzed the complex formation between uranium and 2,3-dihydroxybenzoic acid using the fluorescence properties of the ligand. The formation constant was found to be log K11 = -3.11 ± 0.16.We have validated this complex formation using the fluorescence properties of uranium. The formed complex has no fluorescence properties. This is confirmd by a monoexponetial fluorescence decay and also the fluorescence spectra show no shift in the emission maxima.However the fluorescence lifetime of the non-complexed uranium in the solution depends on the concentration of the added ligand. This is due to the dynamic quench effect of the ligand molecule. This quench effect is strongly correlated to the pH of the solution. This leads to the conclusion that only the protonated ligand effects this quench process. Taking this effect into account we are able to calculate the fluorescence intensities of the non-complexed uranium and by use of these data the complex formation between uranium and 2,3-dihydroxybenzoic acid. We obtained a one to one complex formation accompanied by the release of two protons from the ligand, as also found in the study of the fluorescence properties of the ligand. However the derived complex formation constants differ between both methods. The formation constant obtained from the uranium study was found to be log K = -3.99 ± 0.44. This is about 0.9 orders of magnitude lower compared to the constant derived from the study of the ligand. The confidence limits of the two data sets overlap nevertheless the deviation of the both constants leads to the conclusion that other reactions may be involved. From the uranium fluorescence we do not expect such reactions. But the non-complexed ligand may show separate reactions in the excited state, which lead to a change of the fluorescence intensity of the ligand and resulting in an increase of the calculated formation constant. The consequence of the inclusion of these reactions in the examination leads to an exact determination of the ligand concentration accompanied by a much better agreement of the assigned formation constants.
  • Contribution to proceedings
    Abstract in Proceeding, 21.-26.09.2004, Gyenongiu, Korea
  • Lecture (Conference)
    Migration 03, 22.09.2003, Gyeongiu, Korea

Publ.-Id: 5341 - Permalink

Capability of Surface Complexation Models and Databases for Predicting Radionuclide Sorption
Brendler, V.; Arnold, T.; Richter, A.; Bernhard, G.;
The paper presents examples illustrating the current blind predictive capabilities of surface complexation models (SCM) and respective databases. High-quality experimemtal sorption data sets as provided by Phase II of the NEA Sorption Project for its fitting assessment efforts were used. The systems covered are Np(V) sorption onto hematite, U(VI) sorption onto quartz and Se sorption onto goethite. To keep the number of parameters at a minimum, the Diffuse Double Layer model was selected to account for electrostatics. All calculations were performed with the FITEQL code, version 3.2. Based on the information in the sorption database RES³T [1] for the above minerals and chemically similar phases, first a set of relevant species was formed. Then respective surface complexation parameters were taken from RES³T: the binding site density for the minerals, the surface protolysis constants, and the brutto stability constants for all relevant surface complexes. To be able to compare and average thermodynamic constants originating from different sources, the normalization concept as introduced by Kulik [2] was applied. Lacking data was substituted by estimates exploiting chemical analogy. The only system-specific parameters directly going into the computations were the solid-liquid ratio and the specific surface area.

The model prediction almost always represented the experimental values for the sorbed amount of Np, U and Se, expressed as conventional distribution coefficients KD as required by PA software, within one order of magnitude or better, provided an adequate chemical system was assumed. Further improvements may arise from a broader data base eliminating the need for data estimations through chemical analogies.

[1] RES³T - Rossendorf Expert System for Surface and Sorption Thermodynamics, V. Brendler, A. Vahle, T. Arnold, G. Bernhard, T. Fanghänel, J.Contaminant Hydrology, in press
[2] Sorption modelling by Gibbs energy minimisation: Towards a uniform thermodynamic database for surface complexes of radionuclides. D. Kulik, Radiochim. Acta, 90 (2002), 815-832
  • Lecture (Conference)
    Migration 2003, Sept. Korea

Publ.-Id: 5340 - Permalink

Radiometals for nuclear medicine
Pietzsch, H.-J.; Spies, H.;
Radiometals play an important role in nuclear medicine1-3 for the diagnosis or therapy of various diseases. Beside technetium-99m, the most frequently used radionuclide for in-vivo- diagnosis because its optimal nuclide properties, economically supply by the 99Mo/99mTc generator and easy preparation of the 99mTc-radiopharmaceutical in the clinic, current search for metalloradiopharmaceuticals focuses on both unconventional positron emitting metals (e.g. Cu-64, Ga-66, Y-86, Tc-94m) as potential agents for positron emission tomography (PET) and of radiometal agents labeled with particle emitters for radionuclide therapy3. Since the basic requirement for therapeutic radiopharmaceuticals, namely to induce high effective dose for the target but practically no interference with healthy tissue is not fulfilled yet, the number of therapeutic radiopharmaceuticals for routine use is limited.
Besides the availability of suitable nuclides, the design of chelate systems for stable binding of the radiometal is a crucial point in the development of new metalloradiopharmaceuticals. The chemistry of respective chelates designed in recent years for binding technetium and rhenium at various oxidation states will be discussed. Such chelates involve mixed-ligand complexes containing the metalnitrido core at oxidation state V, Tc(III)/Re(III) and organometallic Tc(I)/Re(I) complexes.
Finally, the application of these chelates for labeling peptides and receptor-affine coordination compounds will be demonstrated.
  • Lecture (Conference)
    18th KAIF/KNS Annual Conference, Korea Atomic Industrial Forum, Inc. (KAIF), Korean Nuclear Society (KNS), Seoul 09.-13.04.2003
  • Lecture (others)
    Korea Cancer Center Hospital Seoul, Dept. Of Nuclear Medicine, 09.04.2003

Publ.-Id: 5339 - Permalink

Tumour specificity of 11C-acetate and 18F-FDG positron emission tomography in prostate cancer patients
Fricke, E.; Machtens, S.; Hofmann, M.; van den Hoff, J.; Bergh, S.; Brunkhorst, T.; Meyer, G. J.; Karstens, J. H.; Knapp, W. H.; Boerner, A. R.;
Visualisation of primary prostate cancer and its metastases remains a clinical important problem, state-of-the-art methods like CT, MRI, TRUS (transrectal ultrasound) and 18F-FDG PET notwithstanding. The difficulties are even more pronounced in case of local recurrence as 18F-FDG PET, while useful in the detection of metastases, is not considered helpful in the investigation of relapse. The aim of this study was to evaluate the efficacy of 11C-acetate and 18F-FDG-PET in the detection of prostate cancer and its metastases in patients treated with or without hormonal ablation.
25 patients (age: 54 to 82 years) were investigated during follow-up of a primary prostate cancer, suspected relapse, or metastatic disease using 11C-acetate PET and 15 with 18F-FDG PET additionally. 14 Patients had antiandrogen treatment at the time of the investigation, the other 11 patients were drug-naive.
Primary tumours were detected in 20/24 (83%) patients using 11C-acetate PET and in 10/15 (75%) patients using 18F-FDG PET. Based on the results of both PET scans, one patient was diagnosed with a lung cancer as second malignancy. Median 18F-FDG uptake exceeded that 11C-acetate in distant metastases (SUV=3.2 vs. 2.3, respectively). 11C-acetate uptake, however, was higher in local recurrence and in local lymph node metastases (median SUVs = 2.9 and 3.8) compared to 11C-acetate (median SUVs = 1.0 and 1.1, respectively). 11C-acetate and 18F-FDG uptake was lower in patients on antiandrogen therapy compared with the drug-naïve patients but 11C-acetate uptake was not significantly impaired. A close correlation of serum PSA level and Gleason score on the one hand and both 11C-acetate uptake and 18F-FDG uptake on the other hand was observed.
These data confirm that 11C-acetate is more useful than 18F-FDG in the detection of local recurrences and localised lymph node metastases. 18F-FDG, however, appears to be more accurate in visualising distant metastases. Antiandrogen therapy reduces tumour metabolic activity and therefore overall PET accuracy but detection of local recurrences by 11C-acetate is not severly compromised. Ultimately, there may be a role for combined 11C-acetate/18F-FDG PET in the follow-up of patients with prostate cancer and persisting or increasing PSA.
Keywords: 11C-acetate PET,18F-FDG PET, prostate cancer, antiandrogen therapy monitoring

Publ.-Id: 5338 - Permalink

Verbesserung des Hochtemperaturoxidationsverhaltens der intermetallischen Verbindung Gamma-TiAl mittels Ionenimplantation
Hornauer, U.;
no abstract
  • Open Access LogoWissenschaftlich-Technische Berichte / Forschungszentrum Rossendorf; FZR-368 März/03


Publ.-Id: 5337 - Permalink

Effect of Secondary FE-Phases
Arnold, T.; Krawczyk-Bärsch, E.; Brandt, F.; Bosbach, D.; Bernhard, G.;
The influence of the formation of secondary iron phases on the sorption behavior of U(VI) on chlorite was investigated in batch sorption experiments with two different types of chlorites: an unaltered chlorite from Flagstaff Hill (CCa-2) and a hydrothermally altered chlorite from Grimsel/Switzerland. The easily extractable ions have not been removed in the CCa-2 chlorite and it therefore tends to form secondary phases. In contrast, the hydrothermally altered chlorite is relative resitant to weathering as discussed in Arnold et. al. [1] and therefore does not tend to form secondary phases. The batch sorption experiments were carried out under ambient temperature and pressure using a solid concentration of 0,5 g chlorite in 40 mL 0,1 M NaClO4 solution. The higher sorption capacity of the unaltered CCa-2 chlorite of more than 20 % of the initially added 1´10-6 M U(VI) compared to the hydrothermally altered chlorite is especially striking in the pH region from 6,5 to 8,5 and was attributed to the generation of secondary Fe and Al phases forming during the two months period of the batch sorption experiments. As a consequence of the formation of a new phase additional mineral surface area is generated [2] which serves as a substrate for further uranium sorption. It is well known that Fe-oxyhydroxide particles show a very high affinity for sorbing U(VI) [3]. Our results clearly show that newly-forming secondary phases may increase the sorption capacity of primary minerals. The Diffuse Double Layer Model (DDLM) was applied to model the U(VI) sorption on the two chlorites including the newly-formed secondary phases.

  • Lecture (Conference)
    Migration 03, Korea Sept. 2003

Publ.-Id: 5336 - Permalink

Fluid Velocity Measurements in Electro-Vortical Flows
Cramer, A.; Gerbeth, G.; Terhoeven, P.; Krätzschmar, A.;
This class of flows is characterized by the feeding of strong electrical currents into a volume of liquid metal. A prominent example of industrial interest is the electrode-welding where the current is supplied via a locally restricted area, leading to high current densities. The interaction of these currents with their own magnetic field drives flows which exhibit phenomena like formation of jets and pinch-effect. Further increasing the current may lead to disruption of the melt column accompanied with a discharge. This can be used for a liquid metal current limiter with self-healing properties.
Local measurements of the flow structures are of obvious interest for a better understanding of these phenomena. The paper will give results from a systematic study of the flow structure performed by means of our mechano-optical velocity probe. The measured flow structure of the evolving jet was found to be in a reasonable agreement with our numerical simulations.
Keywords: Current limiter, electro-vortical flows, pinch effect, measuring techniques for liquid metals, local velocity measurement, local pressure measurement
  • Lecture (Conference)
    132nd Annual Meeting & Exhibition (TMS), San Diego, California, March 2-6, 2003
  • Materials and Manufacturing Processes 19(2004), 665-678

Publ.-Id: 5335 - Permalink

Fluid Flow Measurements in Electrically Driven Vortical Flows
Cramer, A.; Gerbeth, G.; Terhoeven, P.; Krätzschmar, A.;

Passing an electrical current through a volume of conducting fluid drives flow via the interaction with its own magnetic field. Among this class of electro-vortical flows the electrode-welding is a prominent example of industrial interest. In such configurations where a strong current is supplied locally, the resulting high current densities show phenomena like formation of jets and pinch-effect. The latter may disrupt the melt column in the case of very strong currents, accompanied by a discharge. Thus pinching can be used for a liquid metal current limiter with self-healing properties.
Local flow measurements are important for a better understanding of these phenomena. This paper gives results from a systematic study of the fluid motion performed with our mechano-optical velocity probe. The measured flow structure of the evolving jet was found to be in a reasonable agreement with our numerical simulations. Local pressure measurements have been consistent with the experimental and numerical results for the flow field.
  • Lecture (Conference)
    Modelling for Electromagnetic Processing, Hannover, March 24 - 26, 2003. Proceedings pp 241-246, 2003
  • Contribution to external collection
    Modelling for Electromagnetic Processing, Hannover, March 24 - 26, 2003. Proceedings pp 241-246, 2003

Publ.-Id: 5334 - Permalink

Infrared-phonon-polariton resonance of the nonlinear susceptibility in GaAs
Dekorsy, T.; Yakovlev, V. A.; Seidel, W.; Helm, W.; Keilmann, F.;
Nonlinear probing of the fundamental lattice vibration of polar crystals is shown to reveal insight into higher-order cohesive lattice forces. With a free-electron laser tunable in the far infrared we experimentally investigate the dispersion of the second-order susceptibility due to the phonon resonance in GaAs. We observe a strong resonance enhancement of second harmonic light generation at half the optical phonon frequency, and in addition a minimum at a higher frequency below the phonon frequency. Measuring this frequency and comparison to a theoretical model allows the determination of competing higher-order lattice forces.
Keywords: nonlinear optics, SHG, THz, GaAs, phonon-polariton

Publ.-Id: 5331 - Permalink

Tiefenselektive Phasenanalyse in Fe-implantierten GaN-Oberflächen mittels DCEMS
Walterfang, M.; Keune, W.; Reuther, H.;
195-keV Fe+ Ionen wurden mit einer nominellen Dosis von 5x10E16 cmE-2 bei Raumtemperatur in einen GaN(0001)-Wafer implantiert.
  • Poster
    AKF-Frühjahrstagung der DPG, Dresden, 24.-28.3.2003

Publ.-Id: 5329 - Permalink

Aqueous synthesis of derivatized cyclopentadienyl complexes of technetium and rhenium directed towards radiopharmaceutical application
Bernard, J.; Ortner, K.; Spingler, B.; Pietzsch, H.-J.; Alberto, R.;
Half-sandwich complexes of the type (RCOCp)M(CO)3] with M ) Re and 99(m)Tc were synthesized from [M(OH2)3-(CO)3]+ in water. The R group can be an organic residue or a receptor binding biomolecule with a spacer to cyclopentadienyl (Cp). This provides a general route to Cp complexes of technetium without the need for starting from [TcBr(CO)5].
The X-ray structure of [{C6H5CH2COC5H4}Tc(CO)3] has been elucidated. The compound crystallizes in the monoclinic space group P21/c with a = 16.1454(9), b = 7.6300(6), and c = 12.3922(7) Å and beta = 107.792(6)°. We have chosen a serotonergic receptor ligand (WAY) as an example for the derivatization of Cp with a bioactive molecule. WAY is linked to Cp by an aliphatic chain of variable length. The half-sandwich complexes were prepared from water and organic solvents. The structure of [(WAY4-Cp)Re(CO)3] could be elucidated. The compound crystallizes in the monoclinic space group P21/c with a = 15.7112(6), b = 6.8775(3), and c = 25.5217(12) Å and beta = 103.778(5)°. Quantification of inhibition constants gave a clear structure-activity relationship. A single methylene group between the receptor binding site and the half-sandwich complex gave an IC50 of 217 nM for T1A, whereas a butylene linker resulted in retention of the inhibition constant with an IC50 of 6 nM with respect to underivatized WAY. For use as radiopharmaceuticals, the compounds have also been prepared with 99mTc in quantitative yield.
  • Inorganic Chemistry 42 (2003) 1014-1022

Publ.-Id: 5328 - Permalink

Autoradiographic imaging of the serotonin ransporter in the brain of rats and pigs using S-([18F]Fluoromethyl)-(+)-McN5652
Kretzschmar, M.; Brust, P.; Zessin, J.; Cumming, P.; Bergmann, R.; Johannsen, B.;
The [18F]fluoromethyl analogue of (+)-McN5652 ([18F]FMe-McN) has recently been developed as a radioligand for imaging the neuronal serotonin transporter (SERT) with positron emission tomography (PET). We describe here the autoradiographic evaluation of [18F]FMe-McN in the brain of rats and pigs. Autoradiographic studies of [18F]FMe-McN performed on rat and pig brain in vitro showed a high accumulation of radioactivity in the regions rich in SERT, such as amygdala, hypothalamus, superficial gray layer of the superior colliculus, various nuclei of thalamus and substantia nigra. The binding of [18F]FMe-McN was reduced by citalopram, a highly selective inhibitor for SERT. Similar regional specific binding densities of [18F]FMe-McN were observed in both species. The regional distribution and specific binding of this radiotracer correlates well with the distribution and regional brain binding of [3H]citalopram. Region-to-cerebellum ratios of [18F]FMe-McN in vitro reached a maximum value of 20.6 in the rat and 14.5 in the pig. In addition, ex vivo autoradiography of the rat brain was performed 90 min after i.v. administration of [18F]FMe-McN. The highest regional uptake of [18F]FMe-McN was observed in the hypothalamic area, substantia nigra and amygdaloid area. There is a high correlation between the in vitro and in vivo binding. The region-to cerebellum ratio in vivo reached a maximum value of 5.1 in the substantia nigra, the highest yet reported for a 18F-labelled SERT tracer in vivo in this region. Furthermore, the distribution volume of [18F]FMe-McN calculated from the PET data in various regions of the porcine brain is highly correlated with the SERT density as determined by in vitro autoradiography with [3H]citalopram. Thus, [18F]FMe-McN has a clear potential as a radiotracer for studies of the SERT distribution in man with PET.
  • European Neuropsychopharmacology 13 (2003) 387-397

Publ.-Id: 5327 - Permalink

Kühlmittelvermischung in Druckwasserreaktoren - Teil 2, Experimentelle Ausrüstung und Simulation der Vermischung
Grunwald, G.; Höhne, T.; Kliem, S.; Prasser, H.-M.; Richter, K.-H.; Rohde, U.; Weiß, F.-P.;
Das vorliegende Projekt hatte die Ermittlung der räumlichen und zeitlichen Verteilung der Kühlmittelparameter am Spaltzoneneintritt bei transienten Prozessen zum Ziel, bei denen an den einzelnen Kühlmitteleintrittsstutzen des Reaktors Unterschiede in der Borkonzentration bzw. in der Kühlmittel-temperatur auftreten. Die Sicherheitsrelevanz ist durch die Auswirkungen von Deborierungs- und Kaltwassertransienten auf die Leistungsfreisetzung im Reaktorkern gegeben.Mit Hilfe von Experimenten an einem Reaktormodell sowie durch Validierung und Nutzung eines dreidimensionalen Fluidynamikcodes (CFX-4) und durch Entwicklung eines vereinfachten Vermischungsmodells (SAPR) wurden die für die Ermittlung der reaktordynamischen Systemantwort notwendigen Tools zur Beschreibung der Verhältnisse am Kerneintritt geschaffen. Mit der Modellierung der räum-lich und zeitlich aufgelösten Bor- bzw. Temperaturverteilung im RDB wurden die Voraussetzungen für die gekoppelte neutronenkinetisch-thermohydraulische Simulation von Deborierungs- und Kaltwas-sertransienten und deren Sicherheitsbewertung entwickelt. Das Vorhaben beschränkt sich auf Vor-gänge ohne Verdampfung des Kühlmittels, die Vermischung innerhalb des Reaktorkerns bleibt aus-geklammert. Um Mehrfachzirkulationen von Temperatur- bzw. Borkonzentrationsstörungen im Pri-märkreis adäquat abbilden zu können, wurde auch die Vermischung im oberen Plenum behandelt. Zur Lösung der Aufgabe wurde die Versuchsanlage ROCOM (Rossendorf Coolant Mixing Model) aufgebaut. ROCOM ist ein 1:5-Modell eines KONVOI DWR. Durch die volle Abbildung aller vier Um-wälzschleifen, die flexible Versuchssteuerung sowie die speziell für ROCOM entwickelte Gittersen-sormesstechnik zur räumlich und zeitlich hochauflösenden Bestimmung von Konzentrationsverteilungen stellt ROCOM heute eine weltweit führende Versuchsanlage dar. Bei den Experimenten wurden transiente Konzentrationsverteilungen am Kerneintritt für alle gemäß Arbeitsplan zu betrach-tenden Szenarien ermittelt und zur Validierung von CFX-4 genutzt. Das vereinfachte Vermischungs-modell SAPR dient zur effizienten Kopplung zwischen dem thermohydraulischen Systemcode und dem dreidimensionalen neutronenkinetischen Kernmodell.
Keywords: Kühlmittelvermischung, Druckwasserreaktor, Borverdünnungstransienten, Abriss der Frischdampfleitung, Gittersensoren, Konzentrationsmesstechnik, Strömungssimulation
  • Open Access LogoWissenschaftlich-Technische Berichte / Forschungszentrum Rossendorf; FZR-367 Februar 2003


Publ.-Id: 5326 - Permalink

Ellipsometric characterization of ITO films deposited by reactive dual magnetron sputtering
Vinnichenko, M.; Rogozin, A.; Kolitsch, A.; Möller, W.;
Proper characterization of tin doped indium oxide (ITO) films prepared at various deposition parameters is important to produce the layers with low resistivity and high luminous transmittance. Therefore, thin ITO films were grown on insulating substrates by means of pulsed reactive dual magnetron sputtering at different base pressure, magnetron pulse duration and Ar/O2 ratio. To characterize the layers after deposition, spectroscopic ellipsometry (SE) was applied in combination with optical transmittance and resistivity measurements. Surface roughness obtained by SE was corroborated by atomic force microscopy. A significant variation in film deposition rate was observed for experiments with different magnetron pulse duration due to SE results. It agrees with Auger depth profiling data. The latter also showed that the O/In ratio values close to 1.5 correspond to the lowest film resistivity. For ITO films produced at various deposition conditions it was observed that SE derived free electron parameters ratio demonstrates certain minimum. It corresponds to the lowest film resistivity and high transmittance. SE was also applied in situ as a non contact technique to monitor ITO film resistivity optimization during annealing.
Keywords: spectroscopic ellipsometry, tin doped indium oxide, reactive dual magnetron sputtering
  • Lecture (Conference)
    Deutsche Physikalische Gesellschaft (DPG) , Spring Meeting of the Division Condensed Matter Physics in Dresden, 24.03. - 28.03.2003

Publ.-Id: 5325 - Permalink

Spectroscopic ellipsometry application to optimize parameters of ITO films grown by reactive dual magnetron sputtering
Vinnichenko, M. V.; Rogozin, A. I.; Kolitsch, A.; Möller, W.;
Reactive magnetron sputtering provides possibility of high-quality tin doped indium oxide In2O3:Sn (ITO) film deposition on a large substrates at low temperature. Although resistivity and transmittance of ITO films prepared by this technique greatly depend on the deposition parameters [1], which have to be optimized. Unique combination of the ITO properties is controlled by its electronic band structure parameters [2]; the latter can be characterized by optical methods. That is why, this work is focused on application of spectroscopic ellipsometry (SE) for probing of ITO layers.

The ITO films were grown by sputtering of metallic In (90%) - Sn (10%) alloy targets in atmosphere of Ar and O2 mixture by using pulsed dual magnetron system. Base pressure, Ar/O2 ratio and magnetron pulse duration have been varied during the deposition. The films were prepared on Si (100) covered with 500 nm SiO2 and soda lime glass substrates. Spectroscopic ellipsometry was applied within the wavelength range 300-1700 nm in combination with optical transmittance measurements. The spectral dependences of ellipsometric parameters were acquired in autoretarder mode. SE data were fitted simultaneously with transmittance data by using the model of rough graded layer [3] on substrate.

Such approach yielded ITO film thickness and roughness values, which were corroborated by profilometry and atomic force microscopy respectively. A significant variation in film deposition rate was observed only for experiments with different magnetron pulse duration. This parameter is minimal at 50 µs magnetron on-time, than it reaches maximum at 125 µs followed by further decrease at longer pulse durations. Such behavior can be related to changes in plasma density with variation of pulse length that was obtained by Langmuir probe measurements. The film lowest resistivity at high transmittance was achieved at pulse length 100-150 µs. The ITO optical constants were parameterized in Drude-Lorentz approach that permitted to obtain free electron parameters (plasma, wp, and relaxation, wt, frequencies) and interband transition characteristics. Vertical grading of optical constants through the film was quantified. During variation of base pressure, Ar/O2 ratio and pulse duration the minimum values of wt/wp^2 were reached at optimal deposition parameters that provided the lowest resistivity (3.2 mOhm·cm) of the film along with the high transmittance (0.84 for 180 nm thickness). For non optimal deposition parameters the behavior of wt/wp2 ratio qualitatively resembled resistivity dependence. Only in the vicinity of optimal deposition parameters resistivity is proportional to the ratio wt/wp^2 that points on the applicability of free electron approach in this case. For non optimal deposition parameters mechanisms of electric resistivity are more complex and require more detailed investigation of the film structure.

[1] R.B.H. Tahar, T. Ban, Y. Ohya, Y. Takahashi, J. Appl. Phys., 83 (1998) 2631
[2] O.N. Mryasov, A.J. Freeman, Phys. Rev. B, 64 (2001) 233111.
[3] R.A. Synowicki, Thin Solid Films 313-314 (1998) 394.

Keywords: spectroscopic ellipsometry, tin doped indium oxide, reactive dual magnetron sputtering
  • Poster
    11. Bundesdeutsche Fachtagung Plasmatechnologie, 9. - 12. März 2003

Publ.-Id: 5324 - Permalink

Interaction of Desulfovibrio aspöensis with Actinides
Moll, H.; Merroun, M.; Stumpf, T.; Geipel, G.; Selenska-Pobell, S.; Hennig, C.; Rossberg, A.; Bernhard, G.;
Investigations of processes involving actinides and bacteria in environments around nuclear waste repositories are needed for improvement of the scientific basis for performance of safety assessments. Sulfate reducing bacteria (SRB) are of special interest due to their ability to reduce many metals and actinides. Motamedi and Pedersen showed that SRB are frequently distributed in the deep granitic rock aquifers at the Äspö Hard Rock Laboratory (HRL, Sweden) [1]. The presented work is focussed on interactions of curium (III) and uranium (VI) with the strain Desulfovibrio äspöensis, DSM 10631T, recovered from the deep granitic groundwater at the Äspö site [1].
The interaction of D. äspöensis with Cm (III) was investigated by time-resolved laser fluorescence spectroscopy (TRLFS) in the trace concentration range. No evidences were found for changes in the oxidation state of Cm (III). At pH 3, no interaction between Cm (III) and bacteria was detected. With increasing pH, a surface complexation of Cm (III) occurs at the cell walls. The Cm (III)/bacteria surface complex is characterized by its emission spectrum (peak maximum at 600 nm) and its fluorescence emission lifetime (160 ± 15 µs).
80 % of the U (VI), solved initially (0.02 mM) in a liquid medium supplemented with lactate (10 mM) and bacterial biomass (1.10 g/L), was removed by the cells of D. äspöensis after 72 h of incubation at pH 5. Kinetic studies showed that the main amount of U (VI) was removed from the medium during the first 24 h. The microbial activity depended on pH, initial U (VI), and biomass concentration. By using X-ray absorption spectroscopy (XAS), we demonstrated that, in contrast to the above mentioned case with Cm (III), changes of the oxidation state of U (VI) in the precipitate formed by D. äspöensis occurred. The cellular localization of uranium removed from the medium was studied by using Transmission Electron Microscopy (TEM) and Electron-Disperse X-ray (EDX) analyses.

[1] Motamedi, M., Pedersen, K., Int. Syst. Bacteriol. 1998, 48, 311-315.

This work was funded by the BMWi under contract number: 02E9491.The authors are indebted for the use of the 248Cm to the U.S.. Department of Energy, Office of Basic Energy Sciences, through the transplutonium element production facilities at Oak Ridge National Laboratory which was made available as part of a collaboration between FZR and the Lawrence Berkeley National Laboratory (LBNL).
Keywords: Curium, Uranium, Sulfate reducing Bacteria, Desulfovibrio äspöensis, TRLFS, XAS
  • Lecture (Conference)
    MIGRATION '03, 9th International Conference on Chemistry and Migration Behavior of Actinides and Fission Products in the GeosphereGyeongju, Korea September 21 - 26, 2003

Publ.-Id: 5323 - Permalink

Uranium transfer into plants
Günther, A.; Bernhard, G.; Geipel, G.; Rossberg, A.; Reich, T.; Nitsche, H.;
To protect the health of the population, knowledge is necessary about the transfer of radioactive heavy metals, like uranium, via the food chain soil-water-plant-animal-human. The overall process of uptake of heavy elements into plant tissues from contaminated soils is quantified using the soil-to-plant transfer factor (TF). The transfer factor of uranium for lupine and dandelion is in the range of 10-2 to 10-3. To obtain a more mechanistic understanding of the uptake of heavy metals in plants knowledge about the individual physical-chemical processes is needed. This study focuses on the determination of uranium speciation after uptake of uranium by plants (lupine, dandelions, lamb¢s lettuce). For the first time, laser-induced fluorescence spectroscopy and X-ray absorption spectroscopy were used to determine the chemical speciation of uranium in plants. Information on the spatial distribution of uranium in the plant was achieved by scanning electron microscopy, coupled with energy-dispersive X-ray microanalysis. Differences were detected between the uranium speciation in the initial solutions (hydrophonic and pore water of soil) and inside the plants. The oxidation state of uranium remained hexavalent after the uptake. The chemical speciation of uranium was identical in the roots, shoot axis, and leaves and was independent of the various investigated plants. First results are reported concerning the speciation of uranium in cell sap and solid cell components after separation. Spectroscopic data of relevant model compounds (e.g. sugar phosphates, inorganic phosphates, carboxylic acids, proteins) are compared with the uranium complexes in the different compartments of the plants.The results indicate that the uranium is predominantly bound to phosphoryl groups but in dependence on the experimental conditions the formation of uranium carboxylate complexes cannot be excluded.
Keywords: Uranium, Transfer, Plants
  • Poster
    9th Int.Conf. on Chemistry and Migration Behavior of Actinides and Fission Products in the Geosphäre, 21.-26.09.2003, Gyeongju, Korea

Publ.-Id: 5322 - Permalink

Nanodesign durch Ionenstrahlen: Computersimulation, Experiment und Anwendung
Möller, W.;
no abstract
  • Lecture (others)
    TU Wien, Institut für Allgemeine Physik, Austria, Nov. 5, 2002

Publ.-Id: 5321 - Permalink

Ionenimplantation, Plasma-Immersions-Ionenimplantation und ionengestützte Schichtabscheidung
Möller, W.;
no abstract
  • Lecture (others)
    FhI für Werkstoff- und Strahltechnik/TU Dresden, Oct. 15, 2002

Publ.-Id: 5320 - Permalink

Grundlagen der Ionen-Festkörper-Wechselwirkung
Möller, W.;
no abstract
  • Lecture (others)
    Heraeus-Ferienkurs für Physik, TU Dresden, Sept. 16-17, 2002

Publ.-Id: 5319 - Permalink

Selbstorganisierte Nanostrukturen durch Ionenimplantation
Möller, W.;
no abstract
  • Lecture (others)
    Universität Giessen, May 23, 2002

Publ.-Id: 5318 - Permalink

Nanostrukturen durch Ionenimplantation: Computersimulation, Experiment und Anwendung
Möller, W.;
no abstract
  • Lecture (others)
    Universität Stuttgart, Institut für Strahlenphysik, Jan. 24, 2002

Publ.-Id: 5317 - Permalink

Recent developments and prospects of plasma based ion implantation
Möller, W.;
no abstract
  • Lecture (Conference)
    13th International Conference on Surface Engineering, Chengdu, China, Oct. 10-13, 2002

Publ.-Id: 5316 - Permalink

Nanodesign durch Ionenstrahlen
Möller, W.;
no abstract
  • Lecture (Conference)
    Jahrestagung der Deutschen Vakuum-Gesellschaft, Magdeburg, June 20, 2002

Publ.-Id: 5315 - Permalink

Characteristics and applications of plasma immersion ion implantation
Möller, W.;
no abstract
  • Lecture (Conference)
    Workshop "Puls Plasma Surface Technologies", Dresden, June 6, 2002

Publ.-Id: 5314 - Permalink

High-fluence Si-implanted diamond: formation of SiC nanocrystals and sheet resistance
Weishart, H.; Heera, V.; Eichhorn, F.; Pécz, B.; Barna, Á.; Skorupa, W.;
The sheet resistance and structural properties of high-fluence Si-implanted diamond were investigated. In order to minimize the radiation damage and to facilitate SiC formation the implantation was performed at 900 °C. All samples were subsequently annealed in an rf-heated furnace at 1500 °C for 10 minutes in order to remove defects and thermally unstable phases. X-ray diffraction, infrared absorption spectrometry and high-resolution cross-sectional transmission electron microscopy revealed the formation of a buried layer inside the implanted diamond, which contains SiC nanocrystallites. These SiC nanocrystals have a cubic structure and are nearly perfectly aligned with the diamond lattice. Raman spectroscopy was applied to analyze radiation-damage-induced graphitization in dependence on the implantation conditions. The sheet resistance of the samples was measured as function of temperature by four point probe technique in van-der-Pauw geometry. The decrease of the sheet resistance with increasing ion fluence unambiguously shows the influence of implantation-induced damage. The behavior of the sheet resistance can strongly be modified by additional nitrogen implantation The resulting higher conductivity is interpreted as partial incorporation of the nitrogen donor into the SiC nanocrystals. However, when the Si fluence exceeds a critical value of 5.3×1017 Si+cm-2 at 900 °C the diamond is irreversibly damaged and defect related conductivity dominates.
Keywords: silicon carbide (SiC), diamond crystal, ion bombardment, electrical conductivity

Publ.-Id: 5313 - Permalink

Specific Humic Acid Model Substances for the Study of the Redox Behavior of Humic Acids in the Environment
Sachs, S.; Geipel, G.; Heise, K.-H.; Bernhard, G.;
The mobility of actinides in the environment is determined by their speciation which is strongly influenced by their oxidation states. Humic acids (HA) influences the speciation of actinides by complexation. However, they have also significant redox properties which can affect the oxidation states of actinides and consequently their migration in the environment. Thus, it is very important to understand both the complexation and the redox properties of HA in natural systems.
In order to study the redox behavior of HA in more detail we synthesized HA model substances with distinct redox functionalities based on the oxidation of diphenolic compounds in the absence and presence of amino acids. These humic acid-like model substances are characterized by elemental compositions and structural elements that are comparable to natural HA. However, they show phenolic/acidic OH group contents that are higher than those of natural HA. For characterization of the redox properties of these synthetic products, their Fe(III) and ferricyanide redox capacities (RC) were determined at pH 3 and pH 9.2, respectively, and compared to that of purified natural HA from Aldrich. The synthetic products show RC that are up to a factor of 11 and 4 higher than that of Aldrich HA at pH 3 and pH 9.2, respectively. Additionally, we modified, i.e., etherified the phenolic OH groups of these HA by methylation with diazomethane. Applying these modified HA we verified the dominating role of phenolic OH groups in the redox behavior of these HA.
The synthesized HA model substances with distinct redox functionalities are applied to further improve the knowledge on the impact of HA on the redox stability of actinides in the environment. We study the redox stability of uranium(VI) complexes of these HA depending on pH. Uranium(IV) that is formed due to the redox process is spectroscopically determined both directly by laser-induced photoacoustic spectroscopy and indirectly in form of the uranium(IV) arsenazo(III) complex.
Keywords: Humic substances, humic acids, actinides, migration, redox behavior, redox stability, uranium
  • Lecture (Conference)
    9th International Conference on Chemistry and Migration Behavior of Actinides and Fission Products in the Geosphere Migration '03, Gyeongju, Korea, 21.-26.September 2003

Publ.-Id: 5312 - Permalink

Effect of film thickness on a-Si:H properties grown with hydrogen diluted silane
Danesh, P.; Pantchev, B.; Grambole, D.; Schmidt, B.;
a-Si:H films prepared by plasma-enhanced CVD with 10% SiH4 in hydrogen have been studied concerning the effect of film thickness on the hydrogen concentration, interconnected void network and mechanical stress. The hydrogen concentration was determined by nuclear reaction analysis. The interconnected void network was studied by the method of ion exchange in glass substrate. The films were prepared at a substrate temperature in the range of 150 - 270°C. The results show that at the substrate temperature of 150°C the film structure develops as the void network decreases with the film thickness. At the substrate temperature of 270°C the film starts to grow with a dense structure and its structural improvement is manifested by the increase of the intrinsic compressive stress with the film thickness. The hydrogen concentration does not depend on the film thickness at any substrate temperature.
  • Applied Physics Letters, 80 (2002) 2463.

Publ.-Id: 5311 - Permalink

Uptake of Trivalent Actinides (Cm(III)) and Lanthanides (Eu(III)) by Calcium Silicate Hydrates: A Wet Chemistry and Time-Resolved Laser Fluorescence Spectroscopy (TRLFS) Study
Tits, J.; Stumpf, T.; Rabung, T.; Wieland, E.; Fanghänel, T.;

The interaction of the two chemical homologues (Cm (III) and Eu(III)) with calcium silicate hydrates (CSH phases) at pH 13.3 has been investigated in batch-type sorption studies using Eu(III) and complemented with time-resolved laser fluorescence spectroscopy (TRLFS) using Cm(III). The sorption data for Eu(III) reveal fast sorption kinetics and a strong uptake by CSH phases with distribution ratios of (6±3)·105 L kg-1. Three different Cm(III) species have been identified: A non-fluorescing species, which was identified as a curium hydroxide (surface) precipitate, and two fluorescing Cm(III)/CSH sorbed species. The fluorescing sorbed species have characteristic emission spectra with main peak maxima at 618.9 nm and 620.9 nm and fluorescence emission lifetimes of 289 ± 11 µs and 1482 ± 200 µs, respectively. From the fluorescence lifetimes it was calculated that the two fluorescing Cm(III) species have one to two and no water molecules left in their first coordination sphere suggesting that these species are incorporated into the CSH structure. A structural model for Cm(III) and Eu(III) incorporation into CSH phases is proposed based on the substitution for Ca at two different types of sites in the CSH structure.
Key words : curium, europium, CSH, sorption, incorporation, TRLFS

Publ.-Id: 5310 - Permalink

Change of the dipole strength distributions between the neighboring Gamma-soft nuclei 194Pt and 196Pt
Linnemann, A.; von Brentano, P.; Eberth, J.; Enders, J.; Fitzler, A.; Fransen, C.; Guliyev, E.; Herzberg, R.-D.; Käubler, L.; Kuliev, A. A.; von Neumann-Cosel, P.; Pietralla, N.; Prade, H.; Richter, A.; Schwengner, R.; Thomas, H. G.; Weisshaar, D.; Wiedenhöver, I.;
A nuclear resonance fluorescence experiment with two highly efficient EUROBALL Cluster detectors has been performed on the Gamma-soft nucleus 194Pt. Dipole excitations were observed between 2 and 4 MeV excitation energy. They are tentatively interpreted as the main fragments of the scissors mode based on the measurec excitation strengths and a comparison to microscopic calculations in the framework of the quasiparticle random phase approximation (QRPA). The data indicate large differences to the neighbouring isotope 196Pt: a doublingof the observed dipole strength and a shift of the energy centroid by about 600 keV. None of the currently available models is able to reproduce these features consistently in both nuclei.
Keywords: 194Pt(Gamma, Gamma'); Observed dipole strength for E&x;<4MeV; Deduced M1 scissors mode strength and energy centroid; Comparison ton ¹96;Pt
  • Physic letters B 554(2003)15-20

Publ.-Id: 5309 - Permalink

Crack initiation determination for Charpy size specimens
Dzugan, J.;
An investigation in the field of the crack initiation determination for Charpy size specimens was carried out. An extensive literature survey of published methods for the crack initiation was performed. Methods based on the stretch zone width measurement, blunting line, multiple gauge measurement, electric potential drop, compliance changing rate, acoustic emission, ultrasonic method and magnetic emission are discussed in the theoretical part of the report. Analytical methods for the critical J-integral evaluation were also taken into account, as well as the expressions for the J-integral calculation. On the basis of the theoretical survey suitable measurement methods were chosen and applied in the experimental programme to several different materials. Namely blunting line related methods, multiple gauge methods, electric potential drop and compliance changing rate methods were used. The initiation J-integrals were evaluated with use of wide range of evaluation procedures and compared together in order to find a reliable method for the crack initiation determination. There was not found a universal method for the crack initiation determination. The performance of the methods was varying in dependence on the investigated material, so the results enable to choose perspective method for considered case.
  • Open Access LogoWissenschaftlich-Technische Berichte / Forschungszentrum Rossendorf; FZR-366 Februar 2003


Publ.-Id: 5308 - Permalink

Nanocrystals synthesized by ion implantation into single crystals
Eichhorn, F.; Keywords: nanocrystals, x-ray diffraction, structural study, materials research
  • Lecture (Conference)
    13th ESRF Users' Meeting, February 12, 2003 as a short oral presentation

Publ.-Id: 5307 - Permalink

Clonogenic survival of human keratinocytes and rodent fibroblasts after irraditaion with 25 kV X-rays
Panteleeva, A.; Slonina, D.; Brankovic, K.; Spekl, K.; Pawelke, J.; Hoinkis, C.; Dörr, W.;
Low energy X-rays (Eph < 50 keV) are widely used in diagnostic radiology and radiotherapy. However, data on their relative biological effectiveness (RBE) are scarce. Of particular importance for risk estimation are the RBE value of X-rays in the range which is commonly used in mammography (10 - 30 keV). In the present study we have determined clonogenic survival after low-energy X-ray irradiation for 3 cell lines: primary human epidermal keratinocytes (HEKn), mouse fibroblasts (NIH/3T3) and Chinese hamster fibroblasts (V79). Experiments were performed with a 25 kV X-ray tube and compared to 200 kV X-rays as a reference. Compared to the effect of 200 kV X-rays, irradiation with 25 kV X-rays resulted in a decreased survival rate in the murine fibroblasts but not the human epithelial cell line. RBE value was calculated for 10 % surviving fraction. For HEKn cells, RBE was 1.33 ± 0.27, for NIH/3T3 cells 1.25 ± 0.07 and for V79 cells 1.10 ± 0.09. In conclusion, no consistently increased RBE was observed in the various cell lines. Nevertheless, a potential of increased cytogenetic changes has to be considered for risk estimation of low-energy X-rays.

Keywords: Soft X-rays, clonogenic survival, human keratinocytes, rodent fibroblasts, RBE
  • Radiation and Environmental Biophysics 42 (2003) 95-100 Epub 2003 Jun 26.

Publ.-Id: 5305 - Permalink

Institute of Bioinorganic and Radiopharmaceutical Chemistry; Annual Report 2002
Johannsen, B.; Seifert, S.; (Editors)
  • Open Access LogoWissenschaftlich-Technische Berichte / Forschungszentrum Rossendorf; FZR-363 Januar 2003


Publ.-Id: 5304 - Permalink

MBE Growth of (Ga,In)As/Al(As,Sb) MQWs for Intersubband Transition Wavelenghts < 3.5 Micron
Biermann, K.; Böttcher, J.; Künzel, H.; Cronenberg, S.; Grahn, H. T.; Schrottke, L.; Georgiev, N.; Dekorsy, T.; Helm, M.;
Intersubband transitions in InP-based (Ga,In)As/(Al,In)As MQWs cover the wavelength range beyond 3.5 micron. Application of enhanced conduction band edge discontinuity allows for a reduced intersubband transition wavelength. This can be accomplished by replacing (Al,In)As by Al(As,Sb) barriers that can be grown lattice-matched to InP. (Ga,In)As/Al(As,Sb) MQWs were deposited by MBE and characterised using a combination of x-ray diffraction, photoluminescence and IR absorption measurements. Influence of well thickness and doping behaviour were systematically investigated. By
comparison with simplified theoretical calculations, the electronic band structure (interband and intersubband system) was deduced. Based on the corresponding results, the potential of (Ga,In)As/Al(As,Sb) MQWs for implementation in quantum cascade lasers will be discussed.
Keywords: quantum well structure, intersubband transition, X-ray diffraction, photoluminescence, IR absorption spectroscopy
  • Lecture (Conference)
    Deutsche Physikalische Gesellschaft (DPG) -Tagung, Fachverband Halbleiterphysik, HL3.3, Dresden, 2003

Publ.-Id: 5303 - Permalink

A XAS study of the local environments of cations in (U, Ce)O2
Matrin, P.; Ripert, M.; Petit, T.; Reich, T.; Hennig, C.; D'Acapito, F.; Hazemann, J.-L.; Proux, O.;
Mixed Oxide (MOX) fuel is usually considered as a solid solution formed by uranium and plutonium dioxides. Nevertheless, some physico-chemical properties of (U1-y, Puy)O2 samples manufactured under industrial conditions showed anomalies in the domain of plutonium contents ranging between 3 and 15 at.%. Cerium is commonly used as an inactive analogue of plutonium in preliminary studies on MOX fuels. Extended X-ray Absorption Fine Structure (EXAFS) measurements performed at the European Synchrotron Radiation Facility (ESRF) at the cerium and uranium edges on (U1-y, Cey)O2 samples are presented and discussed. They confirmed on an atomic scale the formation of an ideal solid solution for cerium concentrations ranging between 0 and 50 at.%.
  • Journal of Nuclear Materials 312 (2003) 103-110

Publ.-Id: 5301 - Permalink

Double pinhole diffraction of white synchrotron radiation
Leitenberger, L.; Wendrock, H.; Bischoff, L.; Pietsch, U.; Panzer, T.; Grenzer, J.; Pucher, A.;
The spatial coherence of hard X-rays provided by a bending magnet of the storage ring BESSY II was investigated performing Young's interference experiment. The interference pattern was created by the diffraction of two 2 µm pinholes drilled into a thin tantalum foil by focused ion sputtering. Using an energy-dispersive detector with an energy resolution of 200 eV the interference pattern were detected simultaneously between 5 keV < E < 16 keV scanning a 5 µm pinhole through the detector window. The set-up is suitable to characterise the coherence properties of the beamline in a simple manner, i.e. to deduce parameters as the effective source size, the coherence length and the visibility. For the present case the visibility is near 100% at 5 keV and decreases to 20% at 16 keV.
Keywords: double slit experiment, coherent X-rays, white X-ray radiation
  • Lecture (Conference)
    7th. International Conference on X-Ray and Neutron Scattering, Lake Tahoe, California, USA, September 23 - 27, 2002
  • Physica B 336 (2003) 63 - 67

Publ.-Id: 5300 - Permalink

Hard X-ray spatial coherence measurements using a double slit interference
Leitenberger, W.; Wendrock, H.; Bischoff, L.; Pietsch, U.; Panzer, T.; Grenzer, J.;
The spatial coherence of hard X-rays provided by a bending magnet of the storage ring BESSY II was investigated performing Young's interference experiment. The interference pattern was created by the diffraction of two 2 µm pinholes drilled into a thin tantalum foil by focused ion sputtering. Using an energy-dispersive detector with an energy resolution of 200 eV the interference pattern were detected simultaneously between 5 keV < E < 16 keV scanning a 5 µm pinhole through the detector window. The set-up is suitable to characterise the coherence properties of the beamline in a simple manner, i.e. to deduce parameters as the effective source size, the coherence length and the visibility. For the present case the visibility is near 100% at 5 keV and decreases to 20% at 16 keV.
Keywords: double slit experiment, coherent X-rays, white X-ray radiation
  • Lecture (Conference)
    Workshop on Exploiting the Coherence of X-rays, Motzen, Germany, September 23 - 24, 2002

Publ.-Id: 5299 - Permalink

Structure of uranium sorption complexes at monmorillonite edge sites
Hennig, C.; Reich, T.; Dähn, R.; Scheidegger, A. M.;
Extended X-ray absorption fine structure (EXAFS) spectroscopy at the uranium LIII-edge was used for determining the structural environment of aqueous uranyl surbed onto montmorillonite. The study reveals that uranyl uptake at pH~5-~7 and at an initial uranyl concentration of 5x10-5M takes place at amphoteric surface hydroxyl sites as inner-sphere complex. The measured bond distances sites between uranium and the equatorial oxygen atoms are in the range of 2.34 A the presence of a U-Al backscattering pair was determined. This backscattering pair indicates that the binding of the uranyl unit to amphoteric surface hydroxyl sites occurs preferred as a bidentate inner-sphere complex on aluminol groups.
  • Contribution to external collection
    Radiochim. Acta 90, 653-657 (2002), Oldenburg Wissenschaftsverlag, München

Publ.-Id: 5297 - Permalink

Nichtlineare Suszeptibilität von GaAs im THz Frequenzbereich
Dekorsy, T.; Yakovlev, V. A.; Keilmann, F.; Seidel, W.; Helm, M.;
Die nichtlineare Optik im THz Frequenzbereich ist weitgehend unerforscht [1], da hier keine abstimmbaren, intensiven Lichtquellen zur Verfügung stehen. Abstimmbare Freie-Elektronen Laser mit Emissionsfrequenzen im THz Bereich schließen diese Lücke. Wir haben Frequenzverdoppelung unterhalb der optischen Phononresonanz an dünnen GaAs Kristallen mit dem Freie-Elektronen Laser FELIX, Niederlande, durchfgeführt. Erstmals beobachten wir ein Maximum der nichtlinearen Suszeptibilität 2.Ordnung bei der halben Phononfrequenz (4,4 THz) und ein Minimum oberhalb dieser Frequenz (5,3 THz). Dieses Minimum basiert auf einem Vorzeichenwechsel der nichtlinearen Suszeptibilität bedingt durch konkurrierende elektronische und Gitterbeiträge. Ein Vergleich mit Berechnungen [2] zeigt, dass aus der Frequenz dieses Minimums die Beiträge höherer Ordnung des Gitterpotentials zur nichtlinearen Suszeptibilität quantitativ bestimmt werden können [3].

[1] siehe z.B. F. Keilmann, Infr. Phys. 31, 373 (1991).
[2] C. Flytzanis, Phys. Rev. B 6, 1264 (1972).
[3] T. Dekorsy et al. akzepziert zu Phys. Rev. Lett.
Keywords: nonlinear optics, THz, second harmonic generation, phonon-polariton, GaAs
  • Lecture (Conference)
    Frühjahrstagung der Deutschen Physikalischen Gesellschaft, Dresden, 24.-28.3.2003

Publ.-Id: 5296 - Permalink

Focused ion beams from alloy liquid metal ion sources
Bischoff, L.;
An overview of the research activities of the FIB group in the Research Centre
Rossendorf is given. More in detail the fabrication technology of alloy LMIS as well
as their characterization is discussed. The FIB system IMSA-100 is briefly
introduced and typical applications are presented: writing implantation of Co ions
into a heated Si target in order to create maskless sub-micron CoSi2 structures,
bombardment of semiconductor materials with different ions in a wide range of
current density, dose and temperature allows to study the damage creation and
dynamic annealing process.
Keywords: alloy LMIS, FIB system IMSA-100, sub-micron CoSi2 structures,dynamic annealing
  • Lecture (others)
    Seminar, Institute of Solid State Physics and Institute of Electronics, Sofia April 19, 2002

Publ.-Id: 5295 - Permalink

Epitaxial erbium silicide on Ge+ implanted silicon
Travlos, A.; Boukos, N.; Apostolopoulos, G.; Aidinis, C. J.; Bischoff, L.;

Erbium silicide layers were grown epitaxially on Ge+ ion implanted Si. Epitaxy of ErSi2-x layers was achieved at temperature of 750 C.The layers are grown in the tetragonal phase.The growth of the silicide layers resulted in a drastic decrease of the dislocations in the SiGe layer accompanied by the accumulation of defects at the SiGe/ErSi2-x interface.A small redistribution of the Ge in the SiGe layer was also observed.
Keywords: Erbium silicide, Ge+ implantation, SiGe layer
  • Nuclear Instruments and Methods in Physics Research B 196 (2002) 174 - 179

Publ.-Id: 5294 - Permalink

Solidified liquid metal ion sources - formation of a nanoemitter
Knapp, W.; Bischoff, L.; Teichert, J.;
Solidified liquid metal ion sources (LMISs) operating with Au alloy wetted hair-pin emitters can be used as high-intensity electron point sources with nanometer dimension for electron field emission application. A nanoemitter tip on a solidified LMIS emitter can be formed by quenching during ion emission mode. I-V characteristics and the performance of the electron emitting LMIS are presented.
Keywords: liquid metal ion source, electron emitter, quenching, charcteristics
  • Vacuum 69 (2003) 345 - 349

Publ.-Id: 5293 - Permalink

Romanian ancient gold objects studies using nuclear methods
Constantinescu, B.; Cojocaru, V.; Bugoi, R.; Grambole, D.; Herrmann, F.;
The study of trace-elements in archaeological metallic objects can provide important clues about the metal provenance and the involved manufacturing procedures, leading to important conclusions regarding the commercial, cultural and religious exchanges between the antique populations.
Ancient metallic materials are usually inhomogeneous on a scale of 20 microns or less: they contain remains of imperfect smelting, segregated phases in alloys, inclusions.
Due to their exceptional chemical stability, gold artefacts remain essentially unchanged during weathering and aging processes.
Several fragments of ancient gold objects coming from an Eneolithical treasury and from Pietroasa "Closca cu Puii Aur" ("The Golden Brood Hen with ITS Chickens") hoard, unearthed on Romanian territory and two Romanian native gold nuggets samples were analysed using micro-PIXE technique at the Rossendorf TANDETRON microbeam facility.
The purpose of the study was to clarify the metal provenance, establishing if the hypothesis of local gold holds. To reach this goal, trace elements (Cu, Te, Sn, Pb, Hg, As, Zr, Sb) and PEG (Platinum Group Elements) concentrations were determined.
The presence of inclusions (micrometeric size areas of compositions different from surroundings) was also checked. We found some Si, Ca, Fe ones on two Eneolithic samples, and a Ta-Cr one on sample from Pietroasa hoard. The measurements led to conclusions regarding the alluvial origin of the gold for the Eneolithical samples and gave some indications for the possible gold ore sources of Pietroasa treasury, confirming the heterogeneity of this treasury (the two analysed pieces belonged to different stylistic and compositional groups).
21 pieces of gold coins of KOSON type, considered the only kind of gold coins issued by the Daciens, were analysed using EDXRF and PAA (Proton Activation Analysis) methods at Bucharest Institute of Atomic Physics facilities. For EDXRF, three annular excitations sources - Pu 238 (30 mCi), Am 241 (50 mCi) and Am 241 (10 mCi, with nickel window for asorption of soft X-rays) and two X-ray detectors with Be window - a Si(Li) and an HPGe were used. For PAA, each coin was irradiated in vacuum for 5 hours at an incident proton energy of 11 MeV at a current of ca. 50 nA at the 8 MV FN High Voltage Bucharest Tandem and measured using a properly protected Ge(Li) gamma spectrometer. Three groups of coins of different compositions were found, corresponding to simple, complex and no monogram pieces. The gold of Koson coins is not a natural one (electrum) from present Romania's territory, but is similar to the gold of pseudo - Lysimachan staters. Some possible historical conclusions are discussed.
  • Lecture (Conference)
    1st International Symposium on Ancient Gold Technology: America and Europe, 23-25 Oct. 2002 Madrid, Spain

Publ.-Id: 5291 - Permalink

Effect of the fluid convection driven by a rotating magnetic field on the solidification of a PbSn alloy
Willers, B.; Eckert, S.; Michel, U.; Zouhar, G.;
It is already known that the microstructure of a metallic alloy can be affected in a significant way due to the convection in the liquid phase during solidification. A time varying magnetic field can be applied to produce a flow field in the melt which influences the nucleation and growth processes. The aim of our research program is to find a strategy to refine the microstructure of castings by an optimal combination of magnetic field intensity, field frequency and cooling rate. Furthermore, the basic mechanisms controlling the solidification by magnetic fields are investigated.
A cylindrical crucible with a diameter of 50 mm was used to contain the Pb85wt%Sn alloy. A melt height of 60 mm was chosen. The container bottom is positioned on a water cooled copper chill allowing a directed solidification by a vertical heat flux. A rotating magnetic field was generated by an inductor system with 6 coils.
Local temperatures were determined during the solidification process using a set of thermocouples. Cooling curves measured at different locations inside the sample reveal the significant influence of the electromagnetic convection on the local heat transfer. Profiles of the melt velocity were obtained applying the ultrasonic Doppler method..
The Pb-85wt%Sn alloy shows a microstructure with primary tin-crystallites and eutectic. Specimens solidified without a rotating magnetic field showed a columnar dendritic microstructure which is orientated in heat flux direction. The tin crystallites and the eutectic are homogeneously distributed over the whole sample. If the alloy solidifies in a rotating magnetic field the microstructure changes. The shape of the dendrites changes from columnar to equiaxed in direction from the bottom to the top of the specimen and in the same direction the volume content of the eutectic increases.

Keywords: solidification, dendritic growth, convection, rotating magnetic field
  • Lecture (Conference)
    EUROMAT 2003, Lausanne, 01.-05.09.2003
  • Contribution to external collection
    Dieter M. Herlach: Solidification and Crystallization, Weinheim: WILEY-VCH, 2004, 3-527-31011-8, 194-203

Publ.-Id: 5290 - Permalink

Effect of Fe and Ni ion implantation on the magnetoresistance of La(0.7)Sr(0.3)MnO(3)
Vlakhov, E. S.; Wieser, E.; Nenkov, K. A.; Groetzschel, R.;
By low dose ion implantation the magnetoresistance of LSMO is enhanced and the temperature of its maximum is shifted to lower values. At implantation of higher doses the LSMO films become semiconducting.
  • Lecture (Conference)
    European Conference Physics of Magnetism ' 02, Poznan, Poland, July 1-5, 2002
  • phys. stat. sol. (a) 196 (2003) 125-128

Publ.-Id: 5289 - Permalink

Investigation of the effect of irradiation with gaseous and metallic ions on the atomic structure of the alloy Fe+15 at.% Cr
Ovchinnikov, V. V.; Goloborodski, B. Y.; Gushchina, N. V.; Chemerinskaya, L. S.; Semionkin, V. A.; Wieser, E.; Möller, W.;
In the metastable solid solution Fe-15at.%Cr short range ordering (decomposition) was caused by irradiation at 723 K using Ar and Fe ions. The short range order parameter was evaluated from Moessbauer spectra. The short range order caused by the irradiation is much higher compared to the effect of only annealing at723 K for the same time without irradiation. The decomposition is not limited to the penetration depth of the ions but extends over the whole sample thickness of 30 µm. Therefore it is explained as due to radiation dynamic long range effects.
  • Lecture (Conference)
    III International Scientific Conference "Radiation Thermal Effects and Processing in Inorganic Materials", Tomsk, Russia, July 29 - August 03, 2002

Publ.-Id: 5288 - Permalink

Complex Formation between Uranium(VI) and alpha-D-Glucose 1-phosphate
Koban, A.; Geipel, G.; Bernhard, G.;
The complex formation of uranium(VI) with alpha-D-glucose 1-phosphate (C6H11O6PO32-, G1P) was determined by time-resolved laser-induced fluorescence spectroscopy (TRLFS) at pH 4 and potentiometric titration in the pH range from 3 to 10. Both measurements show the formation of a 1:1 complex at lower pH values. The formation constant of UO2(C6H11O6PO3) was calculated from TRLFS measurements to be log beta11 = 5.72 ± 0.12, and from potentiometric titration log beta11 = 5.40 ± 0.25, respectively.
It was found by potentiometric titration that at higher pH values the complexation changes to a 1:2 complex. The stability constant for this complex was calculated to be log beta12 = 8.96 ± 0.18.

Keywords: Uranium, glucose 1-phosphate, complex formation, potentiometric titration, time-resolved laser-induced fluorescence spectroscopy
  • Radiochimica Acta 91 (2003) 393-396

Publ.-Id: 5287 - Permalink

Migration Case Study: Uranium Mining Waste Rock Pile No. 250 in the Region Schlema/Alberoda (Saxony, Germany)
Schmeide, K.; Geipel, G.; Heise, K. H.; Bernhard, G.;
The overall objective of the EC project "Humic Substances in Performance Assessment of Nuclear Waste Disposal: Actinide and Iodine Migration in the Far-Field" is the determination of the effect of humic substances on the actinide migration in natural systems to assess their impact on the long-term safety of radioactive waste repository sites and abandoned uranium mines. This task includes also the implementation of the present knowledge to real existing natural systems thereby verifying the correlation between important parameters, evaluating their environmental impact and finally, uncovering issues not addressed so far.
Uranium mining waste rock piles in the southern parts of the former East Germany represent a significant long-term environmental concern and liability. Although the uranium mines were decommissioned with the end of the uranium ore production in 1990, the legacy of forty-five years of uranium mining, such as abandoned mines, huge waste rock piles and mill tailings, represents a permanent reservoir and source of radioactive and non-radioactive contaminants. The discharge of radionuclides from the waste rock piles and contamination of the surrounding geosphere has to be minimized.
For the case study presented in this paper, the uranium mining waste rock pile no. 250 in Schlema/Alberoda (Saxony, Germany) was chosen. In many respects, this pile resembles other rock piles of this region. The site is characterized comprehensively with regard to composition and activity inventory of rock material and seepage water, uranium species occurring in the seepage water, TOC content and much more. Some important data of other uranium mining waste rock piles that were located in the vicinity of the rock pile no. 250 are also included in this study, especially the fulvic and humic acid content in the seepage water of rock piles and their loading with uranium. The data presented in this natural system study constitute the basis of performance assessment modeling.
Keywords: Transport, Fulvic acid, Humic acid, Uranium, Mine pile
  • Contribution to external collection
    FZKA 6800, Wissenschaftliche Berichte, Forschungszentrum Karlsruhe, Karlsruhe 2003, pp. 79-98.

Publ.-Id: 5286 - Permalink

Range distributions of low-energy carbon ions: a base for subplantation growth models
Neumaier, P.; Dollinger, G.; Bergmaier, A.; Eckstein, W.; Fischer, R.; Görgens, L.; Hofsäss, H.; Jäger, H. U.; Kröger, H.; Ronning, C.;
Range distributions of carbon ions deposited onto tetrahedral amorphous carbon films at kinetic energies between 22 eV and 692 eV are measured utilizing high-resolution elastic recoil detection. These data are compared to range calculations based on binary collision approximation as well as to classical molecular dynamics simulations. Asymmetric range profiles, differences in mean ion ranges and increased range straggling compared to theories are attributed due to self diffusion during thermal spike as well as to intrinsic surface properties of the carbon samples which have to be considered in subplantation growth models.
  • Lecture (Conference)
    Frühjahrstagung des Arbeitskreises Festkörperphysik der Deutschen Physikalischen Gesellschaft (Fachverband Dünne Schichten, Vortrag DS 12.2), 23.-28. März 2003, Dresden

Publ.-Id: 5285 - Permalink

Project-Group ESRF-Beamline (ROBL-CRG), Bi-Annual Report 2001/2002, Wissenschaftlich-Technische Berichte
Schell, N.; (Editor)
The third report from the Project-Group ESRF-Beamline of the Forschungszentrum Rossendorf covers the period from January 2001 until December 2002. The Rossendorf BeamLine (ROBL) at the European Synchrotron Radiation Facility (ESRF) in Grenoble performed again well during this time - although we had major staff fluctuations, including two times a change in the project-management: Dr. W. Matz became head of the Technical Infrastructure at FZR, and Dr. T. Reich had been offered a professorship at the University of Mainz. We congratulate both of them. In the beamtime used by the FZR and collaborating institutes 77 different experiments were scheduled, while in the ESRF scheduled beamtime 21 experiments were performed by external groups. Additionally, a distinct amount of beamtime was devoted to commissioning of new equipment.

The report is organised in three main parts. The first part contains extendet contributions on results obtaines at ROBL. The second part gives an overview about the general experimental possibilities, scheduled experiments, publications, guests having visited ROBL with support of the EC, an staff information. Finally, the third part collects the experimental reports of the user groups received.
  • Open Access LogoWissenschaftlich-Technische Berichte / Forschungszentrum Rossendorf; FZR-364 Januar 2003


Publ.-Id: 5284 - Permalink

Growth mode and texture development in TiN films during magnetron sputtering – an in situ synchrotron radiation study
Schell, N.; Bottiger, J.; Matz, W.; Chevallier, J.;
For the materials research experimental station of the Rossendorf beamline ROBL at the European Synchrotron Radiation Facility in Grenoble, France, a two magnetron sputter deposition chamber for in situ study of film growth by synchrotron X-ray diffraction and reflectivity was developed. It allows high-quality depositions of compound films and multilayers. Heteroepitaxial layer-by-layer growth of TiN on single crystal MgO(0 0 1) was observed by real-time specular X-ray reflectivity showing characteristic oscillations. The pseudomorphic growth was confirmed by high-resolution TEM micrographs. During growth on amorphous SiO2 on Si(0 0 1) substrates, the microstructural development of TiN films was studied in situ as a function of film thickness. With the deposition parameters chosen, a crossover was observed: grains with a (0 0 2) plane parallel to the film surface dominate at small thicknesses, while, at larger thicknesses, (1 1 1) grains dominate. Recrystallisation was identified as a mechanism that controls this texture development.
Keywords: Thin films; Magnetron sputtering; In situ X-ray scattering; TiN
  • Nucl. Instr. & Meth. B 199 (2003) 133-138

Publ.-Id: 5283 - Permalink

Short-wavelength intersubband transitions in InGaAs/AlAs quantum well
Georgiev, N.; Semtsiv, M.; Dekorsy, T.; Eichhorn, F.; Bauer, A.; Helm, M.; Masselink, W. T.;
InGaAs/AlAs quantum wells (QWs) have the potential for the development of new devices based on intersubband transitions, such as near-infrared detectors, ultra-fast switches and light emitters that operate at the communication wavelength of 1.55 mm.However, the increased strain accommodation in the InGaAs/AlAs system considerably affects the band offsets of these QW structures and the performance of the appropriate devices. We report structural and optical characterization of InxGa1-xAs/AlAs/InyAl1-yAs (x ~ 0.7, y ~ 0.55) QW structures grown on InP substrates. In these structures, we utilize the high conduction band offset provided by AlAs. An increased In content in the wells and in the InyAl1-yAs layers helps to compensate the large AlAs tensile strain. Additionally, the smaller InGaAs band gap results in a shift of the first G-like well subband to lower energies relative to the X-minimum in the barrier layers even in very narrow wells. Intersubband absorption at wavelengths shorter than 2.0 mm is observed in thin single QWs. Also presented are spectra of asymmetric coupled QWs and short-period superlattices.
Keywords: quantum well, strain structures, intersubband transitions
  • Lecture (Conference)
    Deutsche Physikalische Gesellschaft (DPG) - Tagung, Fachverband Halbleiterphysik, HL3.3, Dresden, 2003

Publ.-Id: 5282 - Permalink

Mechanism of degradation of surface hardening at elevated temperature in TiAlV-alloys by in situ synchrotron radiation diffraction
Berberich, F.; Matz, W.; Kreißig, U.; Schell, N.; Mücklich, A.;
The surface hardness of the technically important alloy Ti–6Al–4V (wt.%) can be improved by nitrogen implantation. The structural mechanisms of hardening and of the stability of the improved hardness at elevated temperatures are studied. Ion implanted (II) and plasma immersion ion implanted (PII) samples were used. The formation of small TiN crystallites was detected in the as-implanted state, but only for the II samples a considerable surface hardness increase (factor 3) is observed. The in situ XRD experiments showed, that the TiN phase is stable up to temperatures of 650 °C for both types of implantation. At higher temperature Ti2N is formed which is stable up to 770 °C. ERDA results indicate a diffusion of nitrogen into the bulk material. The redistribution of N is responsible for the hardness changes: a slight decrease for II samples but an improvement by a factor of 2.5 for PII samples. The improvements/degradations of hardness and wear are discussed in correlation with the nitrogen depth distribution below the surface.
Keywords: Synchrotron radiation; Ion implantation; Hardening; Ti–6Al–4V
  • Nuclear Instruments & Methods B 199 (2003) 54-58

Publ.-Id: 5281 - Permalink

Development of nanosystems in TiO2 by ion implantation
Fromknecht, R.; Wang, L. M.; Zhu, S.; Sun, K.; van Veen, A.; van Huis, M. A.; Weimann, T.; Wang, J.; Niemeyer, J.; Eichhorn, F.; Wang, T.;
Au-ions were implanted into TiO2 single crystals with doses ranging from 2x1016Au+/cm2 to 6x1016Au+/cm2 at RT and 1000 K. At RT implanted samples were then thermally annealed at temperatures of 550 K to 1550 K. The Au-atoms precipitate to nanocrystals already during implantation at RT with an average particle size of 1.5 nm. HRTEM investigations revealed that the Au-nanocrystals, embedded in amorphous TiO2 regions, have a broad size and range distribution varying from large sizes in the near surface region to smaller sizes at larger depths. In the annealing process a reorientation of the Au-nanocrystals is observed, with the main effect of a decrease of the (111) peak and an increase of the (200)-peak in the XRD spectra. After annealing at 1000 K the particle size of the highly textured Au-implant was evaluated to ~ 6 nm; this means that during annealing the particles grow, leading to a partially coherent orientation in the disordered TiO2-matrix. Au implantation at RT performed through a metal mask with holes resulted in a narrow size distribution (2-6 nm) of the Au-nanocrystals in the near surface region.
Keywords: Au nanocrystals, ion implantation, rutile, x-ray diffraction
  • Lecture (Conference)
    Deutsche Physikalische Gesellschaft, Frühjahrstagung des Arbeitskreises Festkörperphysik, Dresden, 24.-28.3.2003

Publ.-Id: 5280 - Permalink

Cu gettering in ion implanted and annealed silicon in regions before and beyond the main projected ion range
Kögler, R.; Peeva, A.; Lebedev, A.; Posselt, M.; Skorupa, W.; Özelt, G.; Hutter, H.; Behar, M.;
The strong gettering of Cu atoms in single-crystal Si implanted with 3.5 MeV P+ ions was studied after thermal treatment and contamination with low amount of Cu impurity. Cu decorates the remaining damage generated by ion implantation. Three separate Cu gettering layers were detected by secondary ion mass spectrometry: at the main projected ion range, RP, below RP (RP/2 effect) and beyond RP (trans-RP effect). The defects acting as gettering centers at RP/2 and RP are implantation induced excess vacancies and excess interstitials, respectively. Cu profiles fit very well with depth distributions of excess vacancies and excess interstitials simulated by binary collision model for random and channeled ion incidence. The RP/2 and RP gettering layer are implantation induced, whereas the trans-RP gettering layer is formed by thermal treatment. The Cu accumulation in the trans-RP region increases with increasing temperature and/or with increasing annealing time. The RP/2 effect for P+ implantation was found to be significantly reduced in comparison with Si+ implantation. It completely disappears for higher P+ ion fluences. The obtained results are in agreement with the assumption that interstitials carried by P diffusion are the origin of Cu gettering in the trans-RP region.
Keywords: Ion implantation (61.72.Q), Defect formation and annealing (61.72.C), Indirect evidence of defects (61.72.H), Defect diffusion (66.30.L),Cu gettering (61.72.T).

Publ.-Id: 5279 - Permalink

Atomistic simulation of ion-beam-induced defect production within 100 – 1000 ps after ion impact
Posselt, M.;
The formation and evolution of radiation damage by ion bombardment consists of three stages: (i) atomic displacements during ballistic processes, (ii) formation of a (meta)stable defect structure after fast relaxation, and (iii) long-term thermally activated defect rearrangement, migration, recombination and reduction. The first two stages occur on very short time scales and are hardly accessible by available experimental methods. Atomistic computer simulations can contribute to a better understanding of these processes and of their microscopic mechanisms.
In this talk, a combined simulation method is employed to study a relatively simple case, the defect production by a single ion impact in silicon. Processes in the collision cascade with energy transfers above about 100 eV are treated by computer simulations based on the binary collision approximation (BCA). Classical molecular dynamics (MD) calculations are applied to consider processes in certain parts of the cascade which start with energy transfers less than about 100 eV. Detailed investigations are performed to study the temporal evolution of the defect structure until the beginning of the thermally activated phase, and to determine the damage morphology obtained after the fast relaxation. The influence of nuclear energy deposition and target temperature is discussed. The combination of BCA and MD methods allows the effective calculation of the total number and the depth distribution of different defect species (isolated vacancies and self-intersitials as well as more complex defects) formed on average per incident ion after the fast relaxation processes are finished. The procedure yields more realistic initial conditions for the simulation of post-implantation annealing than hitherto used.

Keywords: computer simulation, defect formation, ion implantation
  • Invited lecture (Conferences)
    20th Int. Conf. on Atomic Collisions in Solids (ICACS 20), Puri, India, Jan. 19-24, 2003 (invited talk)

Publ.-Id: 5278 - Permalink

Betriebserfahrungen beim Batch-Monitoring mit adaptiven Stoff- und Wärmebilanzen
Hessel, G.; Heidrich, J.; Hilpert, R.; Roth, M.; Schmitt, W.; Seiler, T.; Weiß, F.-P.;
In der Feinchemie- und Pharmaindustrie werden Chemikalien kleinerer Menge meistens durch diskontinuierlich geführte Batch-Prozesse hergestellt. Zur Unterstützung des Bedienungspersonals bei der schwierigen Prozessführung von Batch-Reaktoren (Rührkesselreaktoren) wurde ein Online-Monitoring-System (MoSys) entwickelt, das auf adaptiven Stoff- und Wärmebilanzen basiert. Die Industrieerprobung erfolgte im Rahmen eines entwickelten Batch-Informations-Management-Systems (BIMS), das in einem separaten Industrie-PC implementiert und über den Terminalbus in die vorhandene Automatisierungstechnik einer Mehrzweckanlage der Degussa AG eingebunden wurde. Die Betriebserfahrungen von zwei Produktionskampagnen zeigten, dass das BIMS/MoSys stabil und zuverlässig arbeitete und die Konzentrationsprofile gut mit den erwarteten Konzentrationsverläufen übereinstimmten.

Mit BIMS/MoSys sind folgende praktische Nutzanwendungen möglich:

- Einsparung einer chemischen Online-Prozessanalytik,
- Erweiterung und Archivierung des bestehenden Prozesswissens,
- Verbesserung der Produktqualität bei komplexen Batch-Prozessen,
- Optimierung der Prozessführung durch die genauere Ermittlung von Anlagen- und Prozess- Kenngrößen,
- Fehler- und Ursachenanalyse anhand der archivierten Batches,
- Rückverfolgbarkeit von Batches bei Problemen (z. B. Qualitätsbeanstandungen),
- Aufbau eines automatisierten Batch-Reports.

Darüber hinaus können unerwünschte Betriebszustände mit erhöhter Zwischenproduktakkumulation und verringerter Raum-Zeit-Ausbeute frühzeitig erkannt und dadurch rechtzeitig Gegenmaßnahmen eingeleitet werden, um größere Verluste zu vermeiden. Das auf adaptiven Stoff- und Wärmebilanzen basierende Online-Monitoring-System ist bei allen ausreichend exothermen ( oder endothermen) Semibatch-Prozessen einsetzbar, wenn geeignete Informationen in den Stoff- und Wärmebilanzen enthalten sind.
  • Abstract in refereed journal
    Chemie Ingenieur Technik, (75), 8 (2003) 1141

Publ.-Id: 5277 - Permalink

INTERACTION OF URANIUM WITH Desulfovibrio äspöensis (DSM 10631T)
Moll, H.; Merroun, M.; Selenska-Pobell, S.; Bernhard, G.;
The FZR/IRC contributions are focussing on the interactions of actinides with indigenous bacteria in Äspö aquifer. We presenting the first results on interactions of the sulfate-reducing bacterium D. äspöensis (DSM 10631T) with uranium(VI). 80 % of the U(VI), solved initially in a concentration of 0.02 mM in a liquid medium supplemented with lactat (10 mM), was removed by the cells of this strain after 72 h of incubation at pH 5.
Keywords: uranium, desulfovibrio, reduction
  • Other report
    Äspö HRL Annual Report 2002 (2003)

Publ.-Id: 5276 - Permalink

Einführung von Facility Management in einer Forschungseinrichtung, Anforderungen, Probleme, Erfahrungen
Joehnk, P.; Keywords: Facility Management, Forschungseinrichtung
  • Lecture (others)
    Workshop Fa. Heinrich Nickel GmbH am 16.01.2003 in Berlin

Publ.-Id: 5274 - Permalink

New possibilities of characterizing growing sputter-deposited thin films
Schell, N.; Bottiger, J.; Matz, W.; Chevallier, J.; Petersen, J.; Andreasen, K. P.; Jensen, T.;
wird nachgereicht
  • Contribution to proceedings
    Proceedings of 9th Annual International Conference on Composite Engineering (ICCE/9), San Diego, USA, July 1-6, 2002, ed. Hui, D., p. 697-698

Publ.-Id: 5272 - Permalink

Institute of Ion Beam Physics and Materials Research: Annual Report 2002
von Borany, J.; Helm, M.; Jäger, H.-U.; Möller, W.; Wieser, E.; (Editors)
Summary of the scientific activities of the institute in 2002 including selected highlight reports, short research contributions and an extended statistics overview.
  • Open Access LogoWissenschaftlich-Technische Berichte / Forschungszentrum Rossendorf; FZR-362 Januar 2003


Publ.-Id: 5271 - Permalink

Influence of annealing on structural properties of metallic multilayers
Hecker, M.; van Loyen, L.; Tietjen, D.; Schell, N.; Schneider, C. M.;
wird nachgereicht
  • Materials Science Forum 378-381 (2001) 370-375

Publ.-Id: 5270 - Permalink

Thermal stability of grain structure and defects in submicrocrystalline and nanocrystalline nickel
Klemm, R.; Thiele, E.; Holste, C.; Eckert, J.; Schell, N.;
The grain and defect structure of submicrocrystalline and nanocrystalline nickel produced by equichannel angular pressing or by ball milling, respectively, has been studied by isochronal and isothermal annealing experiments, and Xray investigations. A detailed analysis of the thermal stability of the di.erent types of microstructures will be presented.
  • Scripta Materialica 46 (2002) 685-690

Publ.-Id: 5269 - Permalink

Internal strains in single grains of fatigued polycrystalline nickel
Thiele, E.; Bretschneider, J.; Buque, C.; Schell, N.; Schwab, A.; Holste, C.;
Bragg diffraction profiles were measured on single grains of different axial orientation in cyclically deformed Ni polycrystals. Diffraction profile parameters were determined and compared with results from profile measurements on fatigued single crystals, showing the same type of dislocation structure as the grains with corresponding axial orientation. Conclusions are drawn concerning the deformation processes in the grains taking into account the activated slip systems, the dislocation density and long-range residual strains.
  • Materials Science Forum 404-407 (2002) 823-828

Publ.-Id: 5268 - Permalink

Ion beam synthesized nanoclusters for silicon-based light emission
Rebohle, L.; von Borany, J.; Fröb, H.; Gebel, T.; Helm, M.; Skorupa, W.;
Strong blue and violet photoluminescence (PL) and electroluminescence (EL) at room temperature has been achieved from thin SiO2 layers implanted with group IV elements. Thermally grown SiO2 .lms with thicknesses between 130 and 500 nm were implanted with Si, Ge or Sn ions followed by di.erent annealing procedures. Based on PL and PL excitation spectra we tentatively interpret the blue–violet PL as due to a T1- S0 transition of an oxygen deficiency center. The strong EL is well visible with the naked eye and reaches a power e.ciency of up to 5E-3 for Ge. Whereas the EL intensity shows a linear dependence on the injection current for Ge-rich layers, the shape of the EL spectrum remains unchanged. It was found that the I–V characteristics shift to lower applied electric fields with increasing implantation
fuence. Furthermore, it is assumed that the luminescence centers will be excited either by field ionization or by the scattering of hot electrons. Finally, the suitability of ion implanted silicon dioxide layers for optoelectronic applications is discussed.
Keywords: Si, Ge, Sn implanted SiO2; Photoluminescence; Optoelectronic application
  • Nuclear Instruments and Methods in Physics Research B 188 (2002) 28–35

Publ.-Id: 5267 - Permalink

In situ high-temperature synchrotron-radiation diffraction studies of Ni and Co–Ni silicidation processes
Rinderknecht, J.; Prinz, H.; Kammler, T.; Berberich, F.; Zschech, E.;
Silicidation processes in nanoscale Ni and CoNi (5at.% Ni) layers on different silicon substrates were investigated using X-ray diffraction. The phase formation sequences as well as the formation and transition temperatures between 200 and 750°C were studied. The impact of different silicon substrates, i.e., polycrystalline Si and (100) oriented Si single-crystal substrates as well as the impact of different species of dopants (As, P) were analysed. The thermal range of the desired low resistance target phases NiSi and Co(0.95)Ni(0.05)Si(2) was determined. The temperatures for phase formation and phase transitions are significantly lowered on polycrystalline Silicon substrates.
Keywords: Ni silicide; Co–Ni silicides; Phase formation, transition temperatures; Impact of dopants, substrate
  • Microelectronic Engineering 64 (2002) 143-149

Publ.-Id: 5266 - Permalink

Plasma immersion ion implantation of nitrogen in Si: Formation of SiO2, Si3N4 and stressed layers under thermal and sputtering effects
Ueda, M.; Beloto, A. F.; Reuther, H.; Parascandola, S.;
Plasma immersion ion implantation of nitrogen in Si: Formation of SiO2,
Si3N4 and stressed layers under thermal and sputtering effects
  • Surface and Coatings Technology 136 (2001) 244-248

Publ.-Id: 5265 - Permalink

Pages: [1] [2] [3] [4] [5] [6] [7] [8] [9] [10] [11] [12] [13] [14] [15] [16] [17] [18] [19] [20] [21] [22] [23] [24] [25] [26] [27] [28] [29] [30] [31] [32] [33] [34] [35] [36] [37] [38] [39] [40] [41] [42] [43] [44] [45] [46] [47] [48] [49] [50] [51] [52] [53] [54] [55] [56] [57] [58] [59] [60] [61] [62] [63] [64] [65] [66] [67] [68] [69] [70] [71] [72] [73] [74] [75] [76] [77] [78] [79] [80] [81] [82] [83] [84] [85] [86] [87] [88] [89] [90] [91] [92] [93] [94] [95] [96] [97] [98] [99] [100] [101] [102] [103] [104] [105] [106] [107] [108] [109] [110] [111] [112] [113] [114] [115] [116] [117] [118] [119] [120] [121] [122] [123] [124] [125] [126] [127] [128] [129] [130] [131] [132] [133] [134] [135] [136] [137] [138] [139] [140] [141] [142] [143] [144] [145] [146] [147] [148] [149] [150] [151] [152] [153] [154] [155] [156] [157] [158] [159] [160] [161] [162] [163] [164] [165] [166] [167] [168] [169] [170] [171] [172] [173] [174] [175] [176] [177] [178] [179] [180] [181] [182] [183] [184] [185] [186] [187] [188] [189] [190] [191] [192] [193] [194] [195] [196] [197] [198] [199] [200] [201] [202] [203] [204] [205] [206] [207] [208] [209] [210] [211] [212] [213] [214] [215] [216] [217] [218] [219] [220] [221] [222] [223] [224] [225] [226] [227] [228] [229] [230] [231] [232] [233] [234] [235] [236] [237] [238] [239] [240] [241] [242] [243] [244] [245] [246] [247] [248] [249] [250] [251] [252] [253] [254] [255] [256] [257] [258] [259] [260] [261] [262] [263]