Nuclear Forensics: A methodology applicable to Nuclear Security and to Non-Proliferation

Nuclear Security aims at the prevention and detection of and response to, theft, sabotage, unauthorized access, illegal transfer or other malicious acts involving nuclear material". Nuclear Forensics is a key element of nuclear security. Nuclear Forensics is defined as a methodology that aims at re-establishing the history of nuclear material of unknown origin. It is based on indicators that arise from known relationships between material characteristics and process history. Thus, nuclear forensics analysis includes the characterization of the material and correlation with production history. To this end, we can make use of parameters such as the isotopic composition of the nuclear material…

The recoil transfer chamber—An interface to connect the physical preseparator TASCA with chemistry and counting setups

Performing experiments with transactinide elements demands highly sensitive detection methods due to the extremely low production rates (one-atom-at-a-time conditions). Preseparation with a physical recoil separator is a powerful method to significantly reduce the background in experiments with sufficiently long-lived isotopes (t1/2≥0.5 s). In the last years, the new gas-filled TransActinide Separator and Chemistry Apparatus (TASCA) was installed and successfully commissioned at GSI. Here, we report on the design and performance of a Recoil Transfer Chamber (RTC) for TASCA—an interface to connect various chemistry and counting setups with the separator. Nuclear reaction products recoiling o…

Speciation and interactions of plutonium with humic substances and kaolinite in aquifer systems

Abstract The speciation of plutonium (Pu) in contact with humic substances (HS) and kaolinite has been performed in aquifer systems. Mainly the redox behavior, complexation, and sorption of plutonium are discussed here. The redox behavior of Pu(VI) in contact with HS was studied and it was found that Pu(VI) is reduced to Pu(III) and Pu(IV) within a couple of weeks. The complexation constants (log  β LC ) of Pu(III) and Pu(IV) with HS have been determined by means of the ultrafiltration method. Furthermore, the sorption of Pu(III) and Pu(IV) onto kaolinite has been investigated as a function of pH by batch experiments under aerobic and anaerobic conditions.

Uran aus deutschen Nuklearprojekten der 1940er Jahre – eine nuklearforensische Untersuchung

Wir berichten hier uber eine nuklearforensische Analyse verschiedener Uranmaterialien aus deutschen Nuklearprojekten der 1940er Jahre, bei denen Uranmetall in verschiedenen Geometrien verwendet wurde. Mithilfe des 230Th/234U-Isotopenverhaltnisses konnte fur das Metall ein Produktionszeitraum von 1940 bis 1943 bestimmt werden. Die geographische Herkunft des Urans wurde anhand des Spurengehalts an Seltenerdelementen und der Strontium-Isotopenverhaltnisse bestimmt. Die Ergebnisse zeigen, dass das bei den deutschen Nuklearprojekten verwendete Uran aus Minen in der Tschechischen Republik stammt. 236U und 239Pu wurden in Spuren nachgewiesen. Diese entsprechen in etwa der Haufigkeit dieser Isotope…

Studies of the ternary systems humic substances – kaolinite – Pu(III) and Pu(IV)

AbstractThe behaviour of plutonium with respect to its migration in the aquifer has been studied under conditions close to nature. Most relevant under these conditions are Pu(III) and Pu(IV) in contact with humic substances (HS) and minerals. As a model for the host rock, kaolinite (KGa-1b) was chosen. The complexation of Pu(III) and Pu(IV) with Aldrich humic acid (AHA) in aqueous solution at ionic strength 0.1 M was investigated by the ultrafiltration method. The sorption of Pu(III) and Am(III) onto kaolinite (K) as a function of pH and metal-ion concentration was studied under aerobic and anaerobic conditions. The pH edge was found at pH∼5.5 independent of the metal-ion concentration and …

Modeling plutonium sorption to kaolinite: Accounting for redox equilibria and the stability of surface species

Abstract Plutonium with its particularly complex redox chemistry may be thermodynamically stable in the states + III to + VI depending on the redox conditions in the environment. Mineral surfaces can also affect Pu redox speciation. Therefore, the interpretation of Pu sorption data becomes particularly challenging, even for simplified laboratory experiments. The present study focuses on Pu sorption to kaolinite. Am(III), Th(IV), Np(V) and U(VI) literature sorption data are used as analogues for the corresponding Pu redox states to calibrate a simple surface complexation model, and the Nernst formalism is applied. Two independent pH–pe diagrams, one for the kaolinite surface and another for …

Isotope selective ultratrace analysis of plutonium by resonance ionisation mass spectrometry

Abstract Resonance ionisation mass spectrometry (RIMS) is a sensitive and selective method for isotopically resolved ultratrace analysis of long-lived radionuclides. For the routine analysis of plutonium three titanium–sapphire lasers pumped by a pulsed Nd:YAG laser in combination with a time-of-flight mass spectrometer are used. The detection limit of this system is as low as 106–107 atoms for the plutonium isotopes 238Pu to 244Pu. The RIMS technique was applied to investigate the isotopic composition and the content of plutonium in a depleted uranium penetrator as used during the Balkan conflict delivering important information on the origin of the depleted uranium in this type of ammunit…

Attempts to chemically investigate element 112

Summary Two experiments aiming at the chemical investigation of element 112 produced in the heavy ion induced nuclear fusion reaction of 48Ca with 238U were performed at the Gesellschaft für Schwerionenforschung (GSI), Darmstadt, Germany. Both experiments were designed to determine the adsorption enthalpy of element 112 on a gold surface using a thermochromatography setup. The temperature range covered in the thermochromatography experiments allowed the adsorption of Hg at about 35 °C and of Rn at about -180 °C. Reports from the Flerov Laboratory for Nuclear Reactions (FLNR), Dubna, Russia claim production of a 5-min spontaneous fission (SF) activity assigned to 283112 for the 238U(48Ca,3n)…

Cover Picture: Uranium from German Nuclear Power Projects of the 1940s— A Nuclear Forensic Investigation (Angew. Chem. Int. Ed. 45/2015)

Electrodeposition methods in superheavy element chemistry

To prepare electrodeposition experiments with superheavy elements (SHE), their homologs were investigated. In the experiments, various electrode materials and electrolytes were used. Critical potentials (E crit ) where the electrodeposition starts and potentials for the deposition of 50% of the atoms in solution (E 50% ) were determined. Underpotential deposition was observed in most cases. An electrolytic cell for a fast electrochemical deposition was developed and the time for the deposition of 50% of the atoms in solution (t 50% ) was determined. Short lived α-emitting isotopes were produced at Gesellschaft fur Schwerionenforschung (GSI), Darmstadt, transferred to the aqueous phase with …

Titelbild: Uran aus deutschen Nuklearprojekten der 1940er Jahre – eine nuklearforensische Untersuchung (Angew. Chem. 45/2015)

Uranium from German Nuclear Power Projects of the 1940s— A Nuclear Forensic Investigation

Here we present a nuclear forensic study of uranium from German nuclear projects which used different geometries of metallic uranium fuel. Through measurement of the (230)Th/(234)U ratio, we could determine that the material had been produced in the period from 1940 to 1943. To determine the geographical origin of the uranium, the rare-earth-element content and the (87)Sr/(86)Sr ratio were measured. The results provide evidence that the uranium was mined in the Czech Republic. Trace amounts of (236)U and (239)Pu were detected at the level of their natural abundance, which indicates that the uranium fuel was not exposed to any major neutron fluence.

Speciation of the oxidation states of plutonium in aqueous solutions by UV/Vis spectroscopy, CE-ICP-MS and CE-RIMS

For the speciation of the plutonium oxidation states in aqueous solutions, the online coupling of capillary electrophoresis (CE) with inductively coupled plasma mass spectrometry (ICP-MS) has been developed. Depending on the radius/electrical charge ratio, the oxidation states III, IV, V, and VI of plutonium are separated by CE, based on the different migration times through the capillary and are detected by ICP-MS. The detection limit is 20 ppb,i.e.109–1010atoms (10-12–10-13g) for one oxidation state with an uncertainty of the reproducibility of the migration times of ≤1% and ≤5% for the peak area. The redox kinetics of the different plutonium oxidation states in the presence of humic subs…