First-principles study of structural, elastic, electronic, vibrational and thermodynamic properties of uranium aluminides

Mei, Zhi -Gang; Yacout, Abdellatif M.

doi:10.1016/j.commatsci.2018.11.008

Title: First-principles study of structural, elastic, electronic, vibrational and thermodynamic properties of uranium aluminides

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Abstract

The structural, elastic, electronic, vibrational and thermodynamic properties of uranium aluminides UAl_x (x = 2, 3, 4) were studied by density functional theory calculations. The single crystal elastic constants of UAl_x were predicted using the stress-strain method, which were further used to calculate the polycrystalline aggregate properties of UAl_x, including bulk modulus, shear modulus, Young’s modulus, and Poisson’s ratio, etc. The calculated electronic density of states confirm that UAl_x compounds are metallic phases with majority states at the Fermi level contributed by U 5f electrons. The phonon dispersion relations and density of states show that the low frequency acoustic phonon modes of UAl_x are dominated by the lattice vibration of uranium atoms while high frequency optical phonon modes are from the vibration of aluminum atoms. Using quasiharmonic approximation, thermodynamic properties of UAl_x, including Gibbs free energy, entropy, heat capacity, and linear thermal expansion coefficient, were predicted by including both lattice vibrational and thermal electronic contributions. The thermal electronic energy was found to be crucial for the description of the temperature dependence of the thermodynamic properties. In conclusion, the derived Gibbs energy functions of UAl_x are expected to be useful to the thermodynamic modeling of the ternary U-Mo-Al system.

Authors:

^[1]; Yacout, Abdellatif M. ^[1]

Argonne National Lab. (ANL), Argonne, IL (United States)

Publication Date:: Wed Nov 14 00:00:00 EST 2018

Research Org.:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Org.:: USDOE National Nuclear Security Administration (NNSA), Office of Counterterrorism and Counterproliferation

OSTI Identifier:: 1483681

Grant/Contract Number:: AC02-06CH11357

Resource Type:: Accepted Manuscript

Journal Name:: Computational Materials Science

Additional Journal Information:: Journal Volume: 158; Journal Issue: C; Journal ID: ISSN 0927-0256

Publisher:: Elsevier

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; Uranium aluminides; Density function theory calculations; Elastic properties; Thermodynamic properties

Citation Formats


                    Mei, Zhi -Gang, and Yacout, Abdellatif M. First-principles study of structural, elastic, electronic, vibrational and thermodynamic properties of uranium aluminides.  United States: N. p., 2018. 
Web.  doi:10.1016/j.commatsci.2018.11.008.

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                    Mei, Zhi -Gang, & Yacout, Abdellatif M. First-principles study of structural, elastic, electronic, vibrational and thermodynamic properties of uranium aluminides.  United States.  https://doi.org/10.1016/j.commatsci.2018.11.008

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                    Mei, Zhi -Gang, and Yacout, Abdellatif M. Wed .  
"First-principles study of structural, elastic, electronic, vibrational and thermodynamic properties of uranium aluminides".  United States.  https://doi.org/10.1016/j.commatsci.2018.11.008.  https://www.osti.gov/servlets/purl/1483681.

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@article{osti_1483681,

  title        = {First-principles study of structural, elastic, electronic, vibrational and thermodynamic properties of uranium aluminides},

  author       = {Mei, Zhi -Gang and Yacout, Abdellatif M.},

  abstractNote = {The structural, elastic, electronic, vibrational and thermodynamic properties of uranium aluminides UAlx (x = 2, 3, 4) were studied by density functional theory calculations. The single crystal elastic constants of UAlx were predicted using the stress-strain method, which were further used to calculate the polycrystalline aggregate properties of UAlx, including bulk modulus, shear modulus, Young’s modulus, and Poisson’s ratio, etc. The calculated electronic density of states confirm that UAlx compounds are metallic phases with majority states at the Fermi level contributed by U 5f electrons. The phonon dispersion relations and density of states show that the low frequency acoustic phonon modes of UAlx are dominated by the lattice vibration of uranium atoms while high frequency optical phonon modes are from the vibration of aluminum atoms. Using quasiharmonic approximation, thermodynamic properties of UAlx, including Gibbs free energy, entropy, heat capacity, and linear thermal expansion coefficient, were predicted by including both lattice vibrational and thermal electronic contributions. The thermal electronic energy was found to be crucial for the description of the temperature dependence of the thermodynamic properties. In conclusion, the derived Gibbs energy functions of UAlx are expected to be useful to the thermodynamic modeling of the ternary U-Mo-Al system.},

  doi          = {10.1016/j.commatsci.2018.11.008},

  journal      = {Computational Materials Science},

  number       = C,

  volume       = 158,

  place        = {United States},

  year         = {Wed Nov 14 00:00:00 EST 2018},

  month        = {Wed Nov 14 00:00:00 EST 2018}

}

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