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Title: Density-functional theory for plutonium

Abstract

We review here developments in the theoretical description and understanding of plutonium in terms of a metal with itinerant (band) 5f electrons. Within this picture most facets of this remarkable and anomalous material are accurately described by first-principle, parameter-free, density-functional-theory (DFT) calculations. We show that the model explains plutonium’s phase stability, elasticity, lattice vibrations, electronic structure, alloy properties, and magnetism. Fluctuations are addressed by means of constrained DFT calculations and new light is shed on the anomalous properties of δ plutonium, including explaining its negative thermal expansion. Effects of alloying and point defects in plutonium are also addressed. It is further emphasized that strong electron correlations, originating from a large intra-atomic Coulomb repulsion (~4 eV) of the 5f electrons, that has often been assumed for plutonium in the literature, is inconsistent with the experimental phase diagram of plutonium.

Authors:
 [1];  [1];  [1]
  1. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Physics Dept.
Publication Date:
Research Org.:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE; LLNL Laboratory Directed Research and Development (LDRD) Program
OSTI Identifier:
1512634
Report Number(s):
LLNL-JRNL-764803
Journal ID: ISSN 0001-8732; 954488
Grant/Contract Number:  
AC52-07NA27344
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Advances in Physics
Additional Journal Information:
Journal Volume: 68; Journal Issue: 1; Journal ID: ISSN 0001-8732
Country of Publication:
United States
Language:
English
Subject:
plutonium; density-functional theory; phase stability; elasticity; electronic structure; magnetism; alloys; defects

Citation Formats

Söderlind, Per, Landa, A., and Sadigh, B. Density-functional theory for plutonium. United States: N. p., 2019. Web. doi:10.1080/00018732.2019.1599554.
Söderlind, Per, Landa, A., & Sadigh, B. Density-functional theory for plutonium. United States. doi:10.1080/00018732.2019.1599554.
Söderlind, Per, Landa, A., and Sadigh, B. Tue . "Density-functional theory for plutonium". United States. doi:10.1080/00018732.2019.1599554.
@article{osti_1512634,
title = {Density-functional theory for plutonium},
author = {Söderlind, Per and Landa, A. and Sadigh, B.},
abstractNote = {We review here developments in the theoretical description and understanding of plutonium in terms of a metal with itinerant (band) 5f electrons. Within this picture most facets of this remarkable and anomalous material are accurately described by first-principle, parameter-free, density-functional-theory (DFT) calculations. We show that the model explains plutonium’s phase stability, elasticity, lattice vibrations, electronic structure, alloy properties, and magnetism. Fluctuations are addressed by means of constrained DFT calculations and new light is shed on the anomalous properties of δ plutonium, including explaining its negative thermal expansion. Effects of alloying and point defects in plutonium are also addressed. It is further emphasized that strong electron correlations, originating from a large intra-atomic Coulomb repulsion (~4 eV) of the 5f electrons, that has often been assumed for plutonium in the literature, is inconsistent with the experimental phase diagram of plutonium.},
doi = {10.1080/00018732.2019.1599554},
journal = {Advances in Physics},
issn = {0001-8732},
number = 1,
volume = 68,
place = {United States},
year = {2019},
month = {4}
}

Journal Article:
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Works referenced in this record:

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