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Theoretical Studies of Spectral Properties of Plutonium

Published online by Cambridge University Press:  01 February 2011

Jian-Xin Zhu ,
A.K. McMahan ,
M.D. Jones ,
T. Durakiewicz ,
J.J. Joyce ,
J.M. Wills  and
R.C. Albers
Jian-Xin Zhu
Affiliation:
jxzhu@lanl.gov, Los Alamos National Laboratory, T-11, Theoretical Division, MS B262, Los Alamos, NM, 87545, United States, (505) 6672363, (505) 6654103
A.K. McMahan
Affiliation:
mcmahan4@llnl.gov, Lawrence Livermore National Laboratory, Livermore, CA, 94550, United States
M.D. Jones
Affiliation:
jonesm@ccr.buffalo.edu, University at Buffalo, SUNY, Buffalo, NY, 14260, United States
T. Durakiewicz
Affiliation:
tomasz@lanl.gov, Los Alamos National Laboratory, Los Alamos, NM, 87545, United States
J.J. Joyce
Affiliation:
jjoyce@lanl.gov, Los Alamos National Laboratory, Los Alamos, NM, 87545, United States
J.M. Wills
Affiliation:
jxw@lanl.gov, Los Alamos National Laboratory, Los Alamos, NM, 87545, United States
R.C. Albers
Affiliation:
rca@lanl.gov, Los Alamos National Laboratory, Los Alamos, NM, 87545, United States
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Abstract

By combining the local density approximation (LDA) with dynamical mean field theory (DMFT), we report a systematic analysis of the spectral properties of δ-plutonium with varying 5f occupancy. The LDA Hamiltonian is extracted from a tight-binding (TB) fit to full-potential linearized augmented plane-wave (FP-LAPW) calculations. The DMFT equations are solved by the exact quantum Monte Carlo (QMC) method and the Hubbard-I approximation. We show the strong sensitivity of the spectral properties to the 5f occupancy, which suggests using this occupancy as a fitting parameter in addition to the Hubbard U. By comparing with PES data, we conclude that the “open shell” 5f5 configuration gives the best agreement, resolving the controversy over 5f “open shell” versus “close shell” atomic configurations in δ-Pu.

Keywords

Puelectronic structurePu
Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 1104: Symposium NN – Actinides 2008—Basic Science, Applications and Technology , 2008 , 1104-NN02-07
Copyright
Copyright © Materials Research Society 2008

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