AVS 61st International Symposium & Exhibition
    Actinides and Rare Earths Focus Topic Tuesday Sessions
       Session AC+AS+MI+SA+SS-TuM

Invited Paper AC+AS+MI+SA+SS-TuM1
The Role of the 5f Band and Partial Occupancy in Actinide L3-edge XANES and RXES Measurements

Tuesday, November 11, 2014, 8:00 am, Room 301

Session: Synchrotron Radiation and Laboratory Based Investigations of Actinides and Rare Earths
Presenter: Corwin Booth, Lawrence Berkeley National Laboratory
Authors: C.H. Booth, Lawrence Berkeley National Laboratory
S.A. Medling, Lawrence Berkeley National Laboratory
Y. Jiang, Lawrence Berkeley National Laboratory
J.G. Tobin, Lawrence Livermore National Laboratory
P.H. Tobash, Los Alamos National Laboratory
J.N. Mitchell, Los Alamos National Laboratory
D.K. Veirs, Los Alamos National Laboratory
M.A. Wall, Lawrence Livermore National Laboratory
P.G. Allen, Lawrence Livermore National Laboratory
J.J. Kas, University of Washington
D. Sokaras, SLAC National Accelerator Laboratory
D. Nordlund, SLAC National Accelerator Laboratory
T.-C. Weng, SLAC National Accelerator Laboratory
E.D. Bauer, Los Alamos National Laboratory
Correspondent: Click to Email
Although actinide (An) L3-edge x-ray absorption near-edge structure (XANES) spectroscopy has been very effective in determining An oxidation states in insulating, ionically-bonded materials, such as in certain coordination compounds and mineral systems, the technique fails in systems featuring more delocalized 5f orbitals, especially in metals. Recently, actinide L3-edge resonant x-ray emission spectroscopy (RXES) has been shown to be an effective alternative. This technique is further demonstrated here using a parametrized partial unoccupied density of states method to quantify both occupancy and delocalization of the 5f orbital in alpha-Pu, delta-Pu, PuCoGa5, PuCoIn5, and PuSb2. These new results, supported by FEFF calculations, highlight the effects of strong correlations on RXES spectra and the technique's ability to differentiate between f-orbital occupation and delocalization. Potential temperature-dependent spectral changes in the hidden order compound URu2Si2 and the superconductor PuCoGa5 will be discussed.