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Title: Ground-State and Thermodynamical Properties of Uranium Mononitride from Anharmonic First-Principles Theory

Abstract

We report on an advanced density-functional theory (DFT) approach for investigating the ground-state and thermodynamical properties of uranium mononitride (UN). The electronic structure for UN at zero temperature is obtained from DFT that utilizes the generalized gradient approximation (GGA) for the electron exchange and correlation functional and includes spin-orbit interaction and an extension with orbital polarization. Thermodynamical properties are computed within the quasi-harmonic approximation in the Debye–Grüneisen model while anharmonicity is captured in the self-consistent ab initio lattice dynamics (SCAILD) scheme. Anharmonic phonons have heretofore never been modeled from first-principles for UN but they turn out to be important. The computed free energy compares well with that of a CALPHAD (CALculation of PHAse Diagrams) assessment of available experimental data.

Authors:
 [1];  [1];  [1];  [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:
1578244
Report Number(s):
LLNL-JRNL-787823
Journal ID: ISSN 2076-3417; ASPCC7; 983245; TRN: US2102180
Grant/Contract Number:  
AC52-07NA27344
Resource Type:
Accepted Manuscript
Journal Name:
Applied Sciences
Additional Journal Information:
Journal Volume: 9; Journal Issue: 18; Journal ID: ISSN 2076-3417
Publisher:
MDPI
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; density-functional theory; anharmonicity; thermodynamical properties; actinides; uranium mononitride

Citation Formats

Söderlind, Per, Landa, Alexander, Perron, Aurélien, Sadigh, Babak, and Heo, Tae Wook. Ground-State and Thermodynamical Properties of Uranium Mononitride from Anharmonic First-Principles Theory. United States: N. p., 2019. Web. doi:10.3390/app9183914.
Söderlind, Per, Landa, Alexander, Perron, Aurélien, Sadigh, Babak, & Heo, Tae Wook. Ground-State and Thermodynamical Properties of Uranium Mononitride from Anharmonic First-Principles Theory. United States. https://doi.org/10.3390/app9183914
Söderlind, Per, Landa, Alexander, Perron, Aurélien, Sadigh, Babak, and Heo, Tae Wook. Sun . "Ground-State and Thermodynamical Properties of Uranium Mononitride from Anharmonic First-Principles Theory". United States. https://doi.org/10.3390/app9183914. https://www.osti.gov/servlets/purl/1578244.
@article{osti_1578244,
title = {Ground-State and Thermodynamical Properties of Uranium Mononitride from Anharmonic First-Principles Theory},
author = {Söderlind, Per and Landa, Alexander and Perron, Aurélien and Sadigh, Babak and Heo, Tae Wook},
abstractNote = {We report on an advanced density-functional theory (DFT) approach for investigating the ground-state and thermodynamical properties of uranium mononitride (UN). The electronic structure for UN at zero temperature is obtained from DFT that utilizes the generalized gradient approximation (GGA) for the electron exchange and correlation functional and includes spin-orbit interaction and an extension with orbital polarization. Thermodynamical properties are computed within the quasi-harmonic approximation in the Debye–Grüneisen model while anharmonicity is captured in the self-consistent ab initio lattice dynamics (SCAILD) scheme. Anharmonic phonons have heretofore never been modeled from first-principles for UN but they turn out to be important. The computed free energy compares well with that of a CALPHAD (CALculation of PHAse Diagrams) assessment of available experimental data.},
doi = {10.3390/app9183914},
journal = {Applied Sciences},
number = 18,
volume = 9,
place = {United States},
year = {2019},
month = {9}
}

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