Density-functional theory for plutonium

doi:10.1080/00018732.2019.1599554

This content will become publicly available on April 9, 2020

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:

Söderlind, Per ^[1]; Landa, A. ^[1]; Sadigh, B. ^[1]

Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States). Physics Dept.

Publication Date:: 2019-04-09

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:: 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.

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                    Söderlind, Per, Landa, A., & Sadigh, B. Density-functional theory for plutonium.  United States.  doi:10.1080/00018732.2019.1599554.

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                    Söderlind, Per, Landa, A., and Sadigh, B. Tue .  
        "Density-functional theory for plutonium".  United States.  doi:10.1080/00018732.2019.1599554.

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@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},

  number       = 1,

  volume       = 68,

  place        = {United States},

  year         = {2019},

  month        = {4}

}

Copy to clipboard

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Works referenced in this record:

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journal, October 1996

Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
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Zunger, Alex; Wei, S.-H.; Ferreira, L. G.
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Similar Records

This content will become publicly available on April 9, 2020

Title: Density-functional theory for plutonium

Abstract

Citation Formats

Generalized Gradient Approximation Made Simple journal, October 1996

Ab initiomolecular dynamics for liquid metals journal, January 1993

Self-Consistent Equations Including Exchange and Correlation Effects journal, November 1965

Ab initio molecular-dynamics simulation of the liquid-metal�amorphous-semiconductor transition in germanium journal, May 1994

Inhomogeneous Electron Gas journal, November 1964

Special quasirandom structures journal, July 1990

Generalized Gradient Approximation Made Simple
journal, October 1996

Ab initiomolecular dynamics for liquid metals
journal, January 1993

Self-Consistent Equations Including Exchange and Correlation Effects
journal, November 1965

Ab initio molecular-dynamics simulation of the liquid-metal�amorphous-semiconductor transition in germanium
journal, May 1994

Inhomogeneous Electron Gas
journal, November 1964

Special quasirandom structures
journal, July 1990