AVS 62nd International Symposium & Exhibition | |
Actinides and Rare Earths Focus Topic | Wednesday Sessions |
Session AC+AS+MI-WeA |
Session: | Chemistry and Physics of the Actinides and Rare Earths |
Presenter: | David Shuh, Lawrence Berkeley National Laboratory |
Correspondent: | Click to Email |
Soft X-ray synchrotron radiation methodologies are being developed and employed at the Advanced Light Source (ALS) of Lawrence Berkeley National Laboratory to elucidate the electronic structure of actinide materials. Results from these investigations have begun to provide improved fundamental knowledge that can be used as a scientific basis for the enhanced design of special-purpose actinide materials and the overall understanding of actinide materials. The experimental developments at the ALS have centered on the use of the Molecular Environmental Science (MES) scanning transmission X-ray microscope (STXM) at Beamline 11.0.2 for near-edge X-ray absorption spectroscopy (XAS), and on X-ray emission spectroscopy (XES) at several beamlines, focusing primarily on light atom constituents (C, N, O, F) for ligand K-edge XAS, and on metal-ion centers plus light-atom signals for XES. The spectromicroscopy capabilities of the STXM provide the means to investigate and determine the speciation in actinide materials and environmentally-relevant systems with spatial resolution that reaches to the true nanoscale.
An absolutely critical and key enabling component for all of the soft X-ray investigations is the contribution of theory, that when combined with experiment, has firmly provided more detailed knowledge of electronic structure in actinide materials in terms of orbital composition and mixing, and oxidation state. The highlights of recent investigations of metallocenes at the carbon K-edge and uranyl complexes at the nitrogen K-edge will be highlighted in this respect. The spectromicroscopy attributes of the STXM have enabled the investigation of contaminant speciation in a range of model and real environmental systems. The results of the most recent environmentally-related studies, cesium in clay materials relevant to clean up efforts in Japan, will be presented.
Acknowledgement: Supported by the Director, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences Heavy Element Chemistry Program of the U.S. DOE at LBNL under Contract No. DE-AC02-05CH11231.