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Title: Phonon density of states for α-plutonium from density-functional theory

Abstract

The ground-state α phase of plutonium has an extraordinary 16-atom per cell, monoclinic crystal structure defined by 20 parameters, including the cell dimensions, not dictated by the symmetry. The electronic, magnetic, and elastic properties of this complicated material have been predicted in the past but here we compute its phonon spectra. Employing a density-functional-theory (DFT) model, that is fully relativistic and accounts for orbital–orbital coupling (orbital polarization, OP), we determine the phonon density of states of α-plutonium and find good agreement with inelastic x-ray scattering. The calculated specific heat also compares very favorably with experiment. An analysis of the partial atom-projected phonon spectra suggests that atom type 8, that is located in a more open space of the structure, dominates the intensity at very high phonon frequencies. This feature of the model is essential for a good agreement with the experimental spectra. The satisfactory comparison between theory and experiment for the phonons and specific heat suggests that the DFT (+OP) approach is appropriate and accurate for α-plutonium.

Authors:
 [1];  [1]
  1. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Publication Date:
Research Org.:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1607846
Report Number(s):
LLNL-JRNL-789105
Journal ID: ISSN 2045-2322; 987406
Grant/Contract Number:  
AC52-07NA27344
Resource Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; Physics - Condensed matter physics

Citation Formats

Söderlind, Per, and Yang, Lin H. Phonon density of states for α-plutonium from density-functional theory. United States: N. p., 2019. Web. https://doi.org/10.1038/s41598-019-55343-z.
Söderlind, Per, & Yang, Lin H. Phonon density of states for α-plutonium from density-functional theory. United States. https://doi.org/10.1038/s41598-019-55343-z
Söderlind, Per, and Yang, Lin H. Tue . "Phonon density of states for α-plutonium from density-functional theory". United States. https://doi.org/10.1038/s41598-019-55343-z. https://www.osti.gov/servlets/purl/1607846.
@article{osti_1607846,
title = {Phonon density of states for α-plutonium from density-functional theory},
author = {Söderlind, Per and Yang, Lin H.},
abstractNote = {The ground-state α phase of plutonium has an extraordinary 16-atom per cell, monoclinic crystal structure defined by 20 parameters, including the cell dimensions, not dictated by the symmetry. The electronic, magnetic, and elastic properties of this complicated material have been predicted in the past but here we compute its phonon spectra. Employing a density-functional-theory (DFT) model, that is fully relativistic and accounts for orbital–orbital coupling (orbital polarization, OP), we determine the phonon density of states of α-plutonium and find good agreement with inelastic x-ray scattering. The calculated specific heat also compares very favorably with experiment. An analysis of the partial atom-projected phonon spectra suggests that atom type 8, that is located in a more open space of the structure, dominates the intensity at very high phonon frequencies. This feature of the model is essential for a good agreement with the experimental spectra. The satisfactory comparison between theory and experiment for the phonons and specific heat suggests that the DFT (+OP) approach is appropriate and accurate for α-plutonium.},
doi = {10.1038/s41598-019-55343-z},
journal = {Scientific Reports},
number = 1,
volume = 9,
place = {United States},
year = {2019},
month = {12}
}

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