Charakterisierung der Submicron-Partikel in einem umweltrelevanten Wasser: Stauwasser in einer Kommunalmülldeponie über einem Schlammteich (Tailing) der Uranerzaufbereitung in Freital/Sachsen

Characterization of Submicron Particles in an Environmentally-Relevant Water: Backwater From a Sanitary Landfill on a Uranium Mine Tailing at Freital, Saxony. A strategy for characterizing submicron particles in environmental waters based on filtration, centrifugation and photon correlation spectroscopy (PCS) is proposed. Filtration and centrifugation are not used here as methods for particle characterization but serve merely as techniques of a rough separation of the sample. They are applied as cautiously and non-invasively as possible and are only aimed at separating the sample sufficiently for measurements by primarily PCS. The separation should unmask small particles that scatter little light and divide the sample into populations of particles that have monomodal or bimodal size distributions. In this way, the strategy optimizes subsequent particle-size determinations by PCS and minimizes the influence of sample preparation on the samples. A further essential feature of this strategy is the parallel application of complementary methods for both sample preparation and particle characterization (filtration/centrifugation, PCS/SEM, gravimetry/ICP-MS etc.). This facilitates the validation of results and increases the probability for recognizing artifacts. Based on our experimental experience, a guideline for PCS measurements on low-concentration colloids with the BI 90/Correlator BI 9000 AT system from Brookhaven Instruments Corp. was developed. This guideline is aimed at obtaining autocorrelation functions of sufficiently good photon counting statistics which is crucial in PCS on colloidal solutions poor in particles. A measuring campaign on an environmentally-relevant water (backwater from a sanitary landfill on a uranium mine tailing at Freital, Saxony) showed the presence of about 1 to 2 mg/l of submicron particles having a particle size of 30 to 300 nm and of about 5 mg/l of suspended matter (>1000 nm)

Measurement of actinide neutron cross sections

The maintenance of strong scientific expertise is criticalto the U.S. nuclear attribution community. It is particularly importantto train students in actinide chemistry and physics. Neutroncross-section data are vital components to strategies for detectingexplosives and fissile materials, and these measurements requireexpertise in chemical separations, actinide target preparation, nuclearspectroscopy, and analytical chemistry. At the University of California,Berkeley and the Lawrence Berkeley National Laboratory we have trainedstudents in actinide chemistry for many years. LBNL is a leader innuclear data and has published the Table of Isotopes for over 60 years.Recently, LBNL led an international collaboration to measure thermalneutron capture radiative cross sections and prepared the EvaluatedGamma-ray Activation File (EGAF) in collaboration with the IAEA. Thisfile of 35,000 prompt and delayed gamma ray cross-sections for allelements from Z=1-92 is essential for the neutron interrogation ofnuclear materials. LBNL has also developed new, high flux neutrongenerators and recently opened a 1010 n/s D+D neutron generatorexperimental facility

Gas chemical investigation of hafnium and zirconium complexes with hexafluoroacetylacetone using preseparated short-lived radioisotopes

Volatile metal complexes of the group 4 elements Zr and Hf with hexafluoroacetylacetonate (hfa) have been studied using short-lived radioisotopes of the metals. The new technique of physical preseparation has been employed where reaction products from heavy-ion induced fusion reactions are isolated in a physical recoil separator - the Berkeley Gas-filled Separator in our work - and made available for chemistry experiments. Formation and decomposition of M(hfa)4 (M=Zr, Hf) has been observed and the interaction strength with a fluorinated ethylene propylene (FEP) Teflon surface has been studied. From the results of isothermal chromatography experiments, an adsorption enthalpy of -ΔHa=(57±3)kJ/mol was deduced. In optimization experiments, the time for formation of the complex and its transport to a counting setup installed outside of the irradiation cave was minimized and values of roughly one minute have been reached. The half-life of 165Hf, for which conflicting values appear in the literature, was measured to be (73.9±0.8)s. Provided that samples suitable for α-spectroscopy can be prepared, the investigation of rutherfordium (Rf), the transactinide member of group 4, appears possible. In the future, based on the studies presented here, it appears possible to investigate short-lived single atoms produced with low rates ( e.g. , transactinide isotopes) in completely new chemical systems, e.g. , as metal complexes with organic ligands as used here or as organometallic compound

Lightest Isotope of Bh Produced Via the 209Bi(52Cr,n)260BhReaction

The lightest isotope of Bh known was produced in the new {sup 209}Bi({sup 52}Cr,n){sup 260}Bh reaction at the Lawrence Berkeley National Laboratory's 88-Inch Cyclotron. Positive identification was made by observation of eight correlated alpha particle decay chains in the focal plane detector of the Berkeley Gas-Filled Separator. {sup 260}Bh decays with a 35{sub -9}{sup +19} ms half-life by alpha particle emission mainly by a group at 10.16 MeV. The measured cross section of 59{sub -20}{sup +29} pb is approximately a factor of four larger than compared to recent model predictions. The influences of the N = 152 and Z = 108 shells on alpha decay properties are discussed

Molecular interactions of plutonium(VI) with synthetic manganese-substituted goethite

Plutonium(VI) sorption on the surface of well-characterized synthetic manganese-substituted goethite minerals (Fe1-xMnxOOH) was studied using X-ray absorption spectroscopy. We chose to study the influence of manganese as a minor component in goethite, because goethite rarely exists as a pure phase in nature. Manganese X-ray absorption near-edge structure measurements indicated that essentially all the Mn in the goethite existed as Mn(III), even though Mn was added during mineral synthesis as Mn(II). Importantly, energy dispersive X-ray analysis demonstrated that Mn did not exist as discrete phases and that it was homogeneously mixed into the goethite to within the limit of detection of the method. Furthermore, Mössbauer spectra demonstrated that all Fe existed as Fe(III), with no Fe(II) present. Plutonium(VI) sorption experiments were conducted open to air and no attempt was made to exclude carbonate. The use of X-ray absorption spectroscopy allows us to directly and unambiguously measure the oxidation state of plutonium in situ at the mineral surface. Plutonium X-ray absorption near-edge structure measurements carried out on these samples showed that Pu(VI) was reduced to Pu(IV) upon contact with the mineral. This reduction appears to be strongly correlated with mineral solution pH, coinciding with pH transitions across the point of zero charge of the mineral. Furthermore, extended X-ray absorption fine structure measurements show evidence of direct plutonium binding to the metal surface as an inner-sphere complex. This combination of extensive mineral characterization and advanced spectroscopy suggests that sorption of the plutonium onto the surface of the mineral was followed by reduction of the plutonium at the surface of the mineral to form an inner-sphere complex. Because manganese is often found in the environment as a minor component associated with major mineral components, such as goethite, understanding the molecular-level interactions of plutonium with such substituted-mineral phases is important for risk assessment purposes at radioactively contaminated sites and long-term underground radioactive waste repositories

Transuranic interfacial reaction studies on manganese oxidemineral surfaces

Several DOE sites have been contaminated by transuranicradionuclide (TRU) discharges including neptunium and plutonium. Theirinteraction with the surrounding geological media can affect thetransport and remediation of these radionuclides in the environment.Manganese based minerals, present as minor phases in the vadose zone, canpreferentially sequester TRU over other minerals present in largerquantities. The objective of this project is to understand theinteractions between plutonium and neptunium and manganese oxyhydroxideminerals to predict potential hazards they represent to the environment,as well as to provide important scientific information for the design ofeffective remediation strategies for contaminated DOE sites

Heavy-Ion Irradiation of Thulium(III) Oxide Targets Prepared by Polymer-Assisted Deposition

Thulium(III) oxide (Tm{sub 2}O{sub 3}) targets prepared by the polymer-assisted deposition (PAD) method were irradiated by heavy-ion beams to test the method's feasibility for nuclear science applications. Targets were prepared on silicon nitride backings (thickness of 1000 nm, 344 {micro}g/cm{sup 2}) and were irradiated with an {sup 40}Ar beam at laboratory frame energy of {approx}210 MeV (50 particle nA). The root mean squared (RMS) roughness prior to irradiation is 1.1 nm for a {approx}250 nm ({approx}220 {micro}g/cm{sup 2}) Tm{sub 2}O{sub 3} target, and an RMS roughness of 2.0 nm after irradiation was measured by atomic force microscopy (AFM). Scanning electron microscopy of the irradiated target reveals no significant differences in surface homogeneity when compared to imaging prior to irradiation. Target flaking was not observed from monitoring Rutherford scattered particles as a function of time

Comparison of reactions for the production of 258,257Db: 208Pb(51V,xn) and 209Bi(50Ti,xn)

Excitation functions for the 1n and 2n exit channels of the 208Pb(51V,xn)259-xDb reaction were measured. A maximum cross section of the 1n exit channel of 2070+1100/-760 pb was measured at an excitation energy of 16.0 +- 1.8 MeV. For the 2n exit channel, a maximum cross section of 1660+450/-370 pb was measured at 22.0 +- 1.8 MeV excitation energy. The 1n excitation function for the 209Bi(50Ti,n)258Db reaction was remeasured, resulting in a cross section of 5480+1750/-1370 pb at an excitation energy of 16.0 +- 1.6 MeV, in agreement with previous values [F. P. Hebberger, et al., Eur. Phys. J. A 12, 57 (2001)]. Differences in cross section maxima are discussed in terms of the fusion probability below the barrier