A combined theoretical and experimental study of the effect of microhydration on ionization energies (IEs) of thymine is presented. The experimental IEs are derived from photoionization efficiency curves recorded using tunable synchrotron VUV radiation. The onsets of the PIE curves are 8.85+-0.05, 8.60+-0.05, 8.55+-0.05, and 8.40+-0.05 eV for thymine, thymine mono-, di-, and tri-hydrates, respectively. The computed (EOM-IP-CCSD/cc-pVTZ) AIEs are 8.90, 8.51, 8.52, and 8.35 eV for thymine and the lowest isomers of thymine mono-, di-, and tri-hydrates. Due to large structural relaxation, the Franck-Condon factors for the 0<-- 0 transitions are very small shifting the apparent PIE onsets to higher energies. Microsolvation strongly affects IEs of thymine -- addition of each water molecule reduces the first vertical IE by 0.10-0.15 eV. The adiabatic IE decreases even more (up to 0.4 eV). The magnitude of the effect varies for different ionized states and for different isomers. For the ionized states that are localized on thymine the dominant contribution to the IE reduction is the electrostatic interaction between the delocalized positive charge on thymine and the dipole moment of the water molecule.

Ion exchange modeling was conducted at the Savannah River National Laboratory to compare the performance of two organic resins in support of Small Column Ion Exchange (SCIX). In-tank ion exchange (IX) columns are being considered for cesium removal at Hanford and the Savannah River Site (SRS). The spherical forms of resorcinol formaldehyde ion exchange resin (sRF) as well as a hypothetical spherical SuperLig{reg_sign} 644 (SL644) are evaluated for decontamination of dissolved saltcake wastes (supernates). Both SuperLig{reg_sign} and resorcinol formaldehyde resin beds can exhibit hydraulic problems in their granular (nonspherical) forms. SRS waste is generally lower in potassium and organic components than Hanford waste. Using VERSE-LC Version 7.8 along with the cesium Freundlich/Langmuir isotherms to simulate the waste decontamination in ion exchange columns, spherical SL644 was found to reduce column cycling by 50% for high-potassium supernates, but sRF performed equally well for the lowest-potassium feeds. Reduced cycling results in reduction of nitric acid (resin elution) and sodium addition (resin regeneration), therefore, significantly reducing life-cycle operational costs. These findings motivate the development of a spherical form of SL644. This work demonstrates the versatility of the ion exchange modeling to study the effects of resin characteristics on processing cycles, rates, and cold chemical …

The Linac Coherent Light Source (LCLS) started user commissioning in October of 2009, producing Free Electron Laser (FEL) radiation between 800 eV and 8 keV [1]. The fundamental wavelength of the FEL dominates radiation in the beamlines, but the beam also produces nonnegligible levels of radiation at higher harmonics. The harmonics may be desirable as a source of harder X-rays, but may also contribute backgrounds to user experiments. In this paper we present preliminary measurements of the second and third harmonic content in the FEL. We also measure the photon energy cutoff of the soft X-ray mirrors to determine the extent to which higher harmonics reach the experimental stations. We present preliminary second and third harmonic measurements for LCLS. At low energies (below 1 keV fundamental) we measure less than 0.1% second harmonic content. The second harmonic will be present in the soft X-ray beam line for fundamental photon energies below approximately 1.1 keV. At low and high energies, we measure third harmonic content ranging from 0.5% to 3%, which is consistent with expectations. For both second and third harmonics, experimental work is ongoing. More rigorous analysis of the data will be completed soon.

The United States (U.S.) currently utilizes a once-through fuel cycle where used nuclear fuel (UNF) is stored on-site in either wet pools or in dry storage systems with ultimate disposal in a deep mined geologic repository envisioned. Within the Department of Energy's (DOE) Office of Nuclear Energy (DOE-NE), the Fuel Cycle Research and Development Program (FCR&D) develops options to the current commercial fuel cycle management strategy to enable the safe, secure, economic, and sustainable expansion of nuclear energy while minimizing proliferation risks by conducting research and development of advanced fuel cycles, including modified open and closed cycles. The safe management and disposition of used nuclear fuel and/or nuclear waste is a fundamental aspect of any nuclear fuel cycle. Yet, the routine disposal of used nuclear fuel and radioactive waste remains problematic. Advanced fuel cycles will generate different quantities and forms of waste than the current LWR fleet. This study analyzes the quantities and characteristics of potential waste forms including differing waste matrices, as a function of a variety of potential fuel cycle alternatives including: (1) Commercial UNF generated by uranium fuel light water reactors (LWR). Four once through fuel cycles analyzed in this study differ by varying the assumed expansion/contraction …