Density functional theory study of cerium deuterides

doi:10.1063/1.5044844

Title: Density functional theory study of cerium deuterides

Abstract

Here, we present a density functional theory study of cerium deuterides, varying deuterium content and temperature. Results are discussed in relation to ejecta experiments recently described in [J. Dynam. Mat. Behav. 1, 12 (2017)]. Using quantum molecular dynamics, we calculate diffusion coefficients, radial distribution functions, and heat capacities of these materials. Properties are calculated over temperatures ranging from 500-4000K at near ambient pressure and at 2.37 fold compression. We find that deuterium diffusion occurs rapidly accross this temperature and compression region and that heat capacity calculations are in agreement with approximations made in experiments. For cerium metal, a comparison of self-diffusion coefficient and viscosity with experimental data and analytical models shows excellent agreement. Lastly, we discuss the stucture of cerium deuterides with respect to radial distribution functions and provide fitted equations for diffusion coefficients over temperature.

Authors:

^[1];

^[1]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Publication Date:: 2018-07-03

Research Org.:: Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Sponsoring Org.:: USDOE Laboratory Directed Research and Development (LDRD) Program

OSTI Identifier:: 1565845

Report Number(s):: LA-UR-17-27804
Journal ID: ISSN 0094-243X

Grant/Contract Number:: 89233218CNA000001; AC52-06NA25396

Resource Type:: Accepted Manuscript

Journal Name:: AIP Conference Proceedings

Additional Journal Information:: Journal Volume: 1979; Conference: SHOCK COMPRESSION OF CONDENSED MATTER, St. Louis, MO (United States), 9-14 July 2014; Journal ID: ISSN 0094-243X

Publisher:: American Institute of Physics (AIP)

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; Cerium; Quantum molecular dynamics; diffusion; hydride; viscosity; liquid metal; ejecta

Citation Formats


                    Bjorgaard, Josiah August, Hammerberg, James Edward, and Sheppard, Daniel Glen. Density functional theory study of cerium deuterides.  United States: N. p., 2018. 
        Web.  doi:10.1063/1.5044844.

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                    Bjorgaard, Josiah August, Hammerberg, James Edward, & Sheppard, Daniel Glen. Density functional theory study of cerium deuterides.  United States.  doi:10.1063/1.5044844.

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                    Bjorgaard, Josiah August, Hammerberg, James Edward, and Sheppard, Daniel Glen. Tue .  
        "Density functional theory study of cerium deuterides".  United States.  doi:10.1063/1.5044844.  https://www.osti.gov/servlets/purl/1565845.

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@article{osti_1565845,

  title        = {Density functional theory study of cerium deuterides},

  author       = {Bjorgaard, Josiah August and Hammerberg, James Edward and Sheppard, Daniel Glen},

  abstractNote = {Here, we present a density functional theory study of cerium deuterides, varying deuterium content and temperature. Results are discussed in relation to ejecta experiments recently described in [J. Dynam. Mat. Behav. 1, 12 (2017)]. Using quantum molecular dynamics, we calculate diffusion coefficients, radial distribution functions, and heat capacities of these materials. Properties are calculated over temperatures ranging from 500-4000K at near ambient pressure and at 2.37 fold compression. We find that deuterium diffusion occurs rapidly accross this temperature and compression region and that heat capacity calculations are in agreement with approximations made in experiments. For cerium metal, a comparison of self-diffusion coefficient and viscosity with experimental data and analytical models shows excellent agreement. Lastly, we discuss the stucture of cerium deuterides with respect to radial distribution functions and provide fitted equations for diffusion coefficients over temperature.},

  doi          = {10.1063/1.5044844},

  journal      = {AIP Conference Proceedings},

  number       = ,

  volume       = 1979,

  place        = {United States},

  year         = {2018},

  month        = {7}

}

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DOI: 10.1063/1.5044844

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Works referenced in this record:

Generalized Gradient Approximation Made Simple
journal, October 1996

Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
DOI: 10.1103/PhysRevLett.77.3865

Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996

Kresse, G.; Furthmüller, J.
Computational Materials Science, Vol. 6, Issue 1, p. 15-50
DOI: 10.1016/0927-0256(96)00008-0

Ab initiomolecular dynamics for liquid metals
journal, January 1993

Kresse, G.; Hafner, J.
Physical Review B, Vol. 47, Issue 1, p. 558-561
DOI: 10.1103/PhysRevB.47.558

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996

Kresse, G.; Furthmüller, J.
Physical Review B, Vol. 54, Issue 16, p. 11169-11186
DOI: 10.1103/PhysRevB.54.11169

From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999

Kresse, G.; Joubert, D.
Physical Review B, Vol. 59, Issue 3, p. 1758-1775
DOI: 10.1103/PhysRevB.59.1758

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Title: Density functional theory study of cerium deuterides

Abstract

Citation Formats

Generalized Gradient Approximation Made Simple journal, October 1996

Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set journal, July 1996

Ab initiomolecular dynamics for liquid metals journal, January 1993

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set journal, October 1996

From ultrasoft pseudopotentials to the projector augmented-wave method journal, January 1999

Generalized Gradient Approximation Made Simple
journal, October 1996

Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996

Ab initiomolecular dynamics for liquid metals
journal, January 1993

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996

From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999