Introduction to FirstPrinciples Electronic Structure Methods: Application to Actinide Materials
Abstract
This paper provides an introduction for nonexperts to firstprinciples electronic structure methods that are widely used in condensedmatter physics. Particular emphasis is placed on giving the appropriate background information needed to better appreciate the use of these methods to study actinide and other materials. Specifically, I describe the underlying theory sufficiently to enable an understanding of the relative strengths and weaknesses of the methods. I also explain the meaning of commonly used terminology, including density functional theory (DFT), local density approximation (LDA), and generalized gradient approximation (GGA), as well as linear muffintin orbital (LMTO), linear augmented plane wave (LAPW), and pseudopotential methods. I also briefly discuss methodologies that extend the basic theory to address specific limitations. Finally, I describe a few illustrative applications, including quantum molecular dynamics (QMD) simulations and studies of surfaces, impurities, and defects. I conclude by addressing the current controversy regarding magnetic calculations for actinide materials.
 Authors:
 Publication Date:
 Research Org.:
 Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
 Sponsoring Org.:
 USDOE
 OSTI Identifier:
 899388
 Report Number(s):
 UCRLJRNL221153
TRN: US0701955
 DOE Contract Number:
 W7405ENG48
 Resource Type:
 Journal Article
 Resource Relation:
 Journal Name: Journal of Materials Research, vol. 21, no. 12, December 1, 2006, pp. 29792985
 Country of Publication:
 United States
 Language:
 English
 Subject:
 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; ACTINIDES; APPROXIMATIONS; DEFECTS; ELECTRONIC STRUCTURE; FUNCTIONALS; IMPURITIES; PHYSICS
Citation Formats
Klepeis, J E. Introduction to FirstPrinciples Electronic Structure Methods: Application to Actinide Materials. United States: N. p., 2006.
Web. doi:10.1557/jmr.2006.0371.
Klepeis, J E. Introduction to FirstPrinciples Electronic Structure Methods: Application to Actinide Materials. United States. doi:10.1557/jmr.2006.0371.
Klepeis, J E. Fri .
"Introduction to FirstPrinciples Electronic Structure Methods: Application to Actinide Materials". United States.
doi:10.1557/jmr.2006.0371. https://www.osti.gov/servlets/purl/899388.
@article{osti_899388,
title = {Introduction to FirstPrinciples Electronic Structure Methods: Application to Actinide Materials},
author = {Klepeis, J E},
abstractNote = {This paper provides an introduction for nonexperts to firstprinciples electronic structure methods that are widely used in condensedmatter physics. Particular emphasis is placed on giving the appropriate background information needed to better appreciate the use of these methods to study actinide and other materials. Specifically, I describe the underlying theory sufficiently to enable an understanding of the relative strengths and weaknesses of the methods. I also explain the meaning of commonly used terminology, including density functional theory (DFT), local density approximation (LDA), and generalized gradient approximation (GGA), as well as linear muffintin orbital (LMTO), linear augmented plane wave (LAPW), and pseudopotential methods. I also briefly discuss methodologies that extend the basic theory to address specific limitations. Finally, I describe a few illustrative applications, including quantum molecular dynamics (QMD) simulations and studies of surfaces, impurities, and defects. I conclude by addressing the current controversy regarding magnetic calculations for actinide materials.},
doi = {10.1557/jmr.2006.0371},
journal = {Journal of Materials Research, vol. 21, no. 12, December 1, 2006, pp. 29792985},
number = ,
volume = ,
place = {United States},
year = {Fri May 05 00:00:00 EDT 2006},
month = {Fri May 05 00:00:00 EDT 2006}
}

The purpose of this paper is to provide an introduction for nonexperts to firstprinciples electronic structure methods that are widely used in the field of condensedmatter physics, including applications to actinide materials. The methods I describe are based on density functional theory (DFT) within the local density approximation (LDA) and the generalized gradient approximation (GGA). In addition to explaining the meaning of this terminology I also describe the underlying theory itself in some detail in order to enable a better understanding of the relative strengths and weaknesses of the methods. I briefly mention some particular numerical implementations of DFT, includingmore »

Electronic Structure and Ionicity of Actinide Oxides from First Principles
The groundstate electronic structures of the actinide oxides AO, A{sub 2}O{sub 3}, and AO{sub 2} (A=U, Np, Pu, Am, Cm, Bk, and Cf) are determined from firstprinciples calculations, using the selfinteraction corrected local spindensity approximation. Emphasis is put on the degree of felectron localization, which for AO{sub 2} and A{sub 2}O{sub 3} is found to follow the stoichiometry, namely, corresponding to A{sup 4+} ions in the dioxide and A{sup 3+} ions in the sesquioxides. In contrast, the A{sup 2+} ionic configuration is not favorable in the monoxides, which therefore become metallic. The energetics of the oxidation and reduction in themore » 
Electronic structure and ionicity of actinide oxides from first principles
The groundstate electronic structures of the actinide oxides AO , A _{2} O _{3} , and AO _{2} (A=U , Np, Pu, Am, Cm, Bk, and Cf) are determined from firstprinciples calculations, using the selfinteraction corrected local spindensity approximation. Emphasis is put on the degree of f electron localization, which for AO _{2} and A _{2} O _{3} is found to follow the stoichiometry, namely, corresponding to A ^{4+} ions in the dioxide and A ^{3+} ions in the sesquioxides. In contrast, the A ^{2+} ionic configuration is not favorable in the monoxides, which therefore become metallic. The energetics ofmore »