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Title: Anharmonic properties in M g 2 X ( X = C , Si , Ge , Sn , Pb ) from first-principles calculations

Abstract

Thermal conductivity reduction is one of the potential routes to improve the performance of thermoelectric materials. Yet, detailed understanding of the thermal transport of many promising materials is still missing. In this paper, we employ electronic-structure calculations at the level of density functional theory to elucidate thermal transport properties of the Mg2X (X = C , Si, Ge, Sn, and Pb) family of compounds, which includes M g 2 Si , a material already identified as a potential thermoelectric. All these materials crystallize into the same antifluorite structure. Systematic trends in the anharmonic properties of these materials are presented and examined. These calculations indicate that the reduction in the group velocity is the main driver of the thermal conductivity trend in these materials, as the phonon lifetimes in these compounds are very similar. We also examine the limits of the applicability of perturbation theory to study the effect of point defects on thermal transport and find that it is in good agreement with experiment in a wide range of scattering parameter values. The thermal conductivity of the recently synthesized Mg2C is computed and predicted to be 34 W/mK at 300°C.

Authors:
 [1];  [1]
  1. Univ. of Florida, Gainesville, FL (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Materials Science of Nuclear Fuel (CMSNF)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1369977
Alternate Identifier(s):
OSTI ID: 1209188
Grant/Contract Number:  
AC07-05ID14517
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Physical Review. B, Condensed Matter and Materials Physics
Additional Journal Information:
Journal Volume: 92; Journal Issue: 6; Related Information: CMSNF partners with Idaho National Laboratory (lead); Colorado School of Mines; University of Florida; Oak Ridge National Laboratory; Purdue University; University of Wisconsin at Madison; Journal ID: ISSN 1098-0121
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Chernatynskiy, Aleksandr, and Phillpot, Simon R. Anharmonic properties in Mg2X (X=C,Si,Ge,Sn,Pb) from first-principles calculations. United States: N. p., 2015. Web. doi:10.1103/PhysRevB.92.064303.
Chernatynskiy, Aleksandr, & Phillpot, Simon R. Anharmonic properties in Mg2X (X=C,Si,Ge,Sn,Pb) from first-principles calculations. United States. https://doi.org/10.1103/PhysRevB.92.064303
Chernatynskiy, Aleksandr, and Phillpot, Simon R. 2015. "Anharmonic properties in Mg2X (X=C,Si,Ge,Sn,Pb) from first-principles calculations". United States. https://doi.org/10.1103/PhysRevB.92.064303. https://www.osti.gov/servlets/purl/1369977.
@article{osti_1369977,
title = {Anharmonic properties in Mg2X (X=C,Si,Ge,Sn,Pb) from first-principles calculations},
author = {Chernatynskiy, Aleksandr and Phillpot, Simon R.},
abstractNote = {Thermal conductivity reduction is one of the potential routes to improve the performance of thermoelectric materials. Yet, detailed understanding of the thermal transport of many promising materials is still missing. In this paper, we employ electronic-structure calculations at the level of density functional theory to elucidate thermal transport properties of the Mg2X (X = C , Si, Ge, Sn, and Pb) family of compounds, which includes M g 2 Si , a material already identified as a potential thermoelectric. All these materials crystallize into the same antifluorite structure. Systematic trends in the anharmonic properties of these materials are presented and examined. These calculations indicate that the reduction in the group velocity is the main driver of the thermal conductivity trend in these materials, as the phonon lifetimes in these compounds are very similar. We also examine the limits of the applicability of perturbation theory to study the effect of point defects on thermal transport and find that it is in good agreement with experiment in a wide range of scattering parameter values. The thermal conductivity of the recently synthesized Mg2C is computed and predicted to be 34 W/mK at 300°C.},
doi = {10.1103/PhysRevB.92.064303},
url = {https://www.osti.gov/biblio/1369977}, journal = {Physical Review. B, Condensed Matter and Materials Physics},
issn = {1098-0121},
number = 6,
volume = 92,
place = {United States},
year = {Fri Aug 07 00:00:00 EDT 2015},
month = {Fri Aug 07 00:00:00 EDT 2015}
}

Journal Article:

Citation Metrics:
Cited by: 13 works
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Works referenced in this record:

Density-Functional Perturbation Theory for Quasi-Harmonic Calculations
journal, January 2010


Anharmonic effects in Mg2X (X = Si, Ge, Sn) compounds studied by Raman spectroscopy
journal, January 1987


Ab initio thermal transport in compound semiconductors
journal, April 2013


Lattice thermal conductivity of MgO at conditions of Earth's interior
journal, February 2010


Projector augmented-wave method
journal, December 1994


Lattice Dynamics of Mg 2 Pb at Room Temperature
journal, March 1972


Highly effective Mg 2 Si 1 x Sn x thermoelectrics
journal, July 2006


Phonon-Mediated Thermal Conductivity in Ionic Solids by Lattice Dynamics-Based Methods
journal, July 2011


Elastic constants and calculated lattice vibration frequencies of Mg2Sn
journal, March 1967


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


Lattice dynamics of magnesium stannide at room temperature
journal, May 1970


Bonding in Mg2Si Studied with X-ray Photoelectron Spectroscopy
journal, June 1995


Bipolar Electronic Thermal Conductivity in Semimetals
journal, October 1962


Lattice dynamics of Mg2Ge
journal, December 1965


Melt growth and characterization of Mg2Si bulk crystals
journal, August 2007


In situ X-ray observation of phase transitions in under high pressure
journal, May 2009


Synthesis of Mg 2 C: A Magnesium Methanide
journal, July 2013


Phonon Lifetime Investigation of Anharmonicity and Thermal Conductivity of UO 2 by Neutron Scattering and Theory
journal, April 2013


Vibrational thermodynamics of materials
journal, May 2010


Ab initiomolecular dynamics for liquid metals
journal, January 1993


First-principles studies of intrinsic point defects in magnesium silicide
journal, April 2009


Phonon conduction in PbSe, PbTe, and PbTe 1 x Se x from first-principles calculations
journal, May 2012


Ab initio theory of the lattice thermal conductivity in diamond
journal, September 2009


Phonon Transport Simulator (PhonTS)
journal, July 2015


First-principles investigation of the electronic and lattice vibrational properties of Mg 2 C
journal, October 2014


Thermal conductivity of argon at high pressure from first principles calculations
journal, August 2013


Direct Solution to the Linearized Phonon Boltzmann Equation
journal, June 2013


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


Thermal stability and elastic properties of Mg2X (X=Si, Ge, Sn, Pb) phases from first-principle calculations
journal, January 2012


Raman Scattering in Mg 2 Si, Mg 2 Ge, and Mg 2 Sn
journal, April 1971


Studies on AB2-type intermetallic compounds, I. Mg2Ge and Mg2Sn: single-crystal structure refinement and ab initio calculations
journal, March 1996


Thermoelectric Performance of Sb- and La-Doped Mg2Si0.5Ge0.5
journal, March 2012


Lattice dynamics in intermetallic Mg 2 Ge and Mg 2 Si
journal, November 2014


Mechanochemical synthesis and thermoelectric properties of high quality magnesium silicide
journal, January 2011


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


Thermodynamic properties of Mg2Si and Mg2Ge investigated by first principles method
journal, June 2010


Simple view of the Mg 2 Si 1 x Sn x phonon spectrum: Sn resonances and mean field
journal, February 2015


Thermal study of group II–IV semiconductors—I. Heat capacity of Mg2Ge in the range 5–300°K
journal, June 1966


Thermal conductivity of bulk and nanowire Mg 2 Si x Sn 1 x alloys from first principles
journal, November 2012


Debye temperatures of 24 cubic elements by three methods
journal, October 1969


Thermal conductivity of magnesium plumbide
journal, June 1974


Thermal Study of Groups II—IV Semiconductors. Lattice Heat Capacities and Free Energies of Formation. Heat Capacity of Mg 2 Si from 15°—300°K
journal, September 1967


Infrared Reflectivities of Magnesium Silicide, Germanide, and Stannide
journal, June 1963


Lattice dynamics of Mg2Si and Mg2Ge compounds from first-principles calculations
journal, May 2008


Effective charge on silicon atom in the metal silicides Mg 2 Si and CaSi
journal, May 2005


Magnetron Deposition of In Situ Thermoelectric Mg2Ge Thin Films
journal, February 2009


Thermal study of II–IV semiconductors: Heat capacity and thermodynamic functions of Mg2Pb from 5–300°K
journal, November 1971


Defect and phase stability of solid solutions of Mg2X with an antifluorite structure: An ab initio study
journal, September 2012


X-Ray characteristic temperature and thermal expansion coefficient of Mg2Ge
journal, November 1973


Lattice dynamics of magnesium stannide at room temperature
journal, December 1969


High-resolution X-ray luminescence extension imaging
journal, February 2021


Synthesis of Mg 2 C: A Magnesium Methanide
journal, July 2013


Elastic constants and calculated lattice vibration frequencies of Mg2Sn
journal, November 1966


Ab initio theory of the lattice thermal conductivity in diamond
text, January 2009


Works referencing / citing this record:

Thermoelectric and vibrational properties of Be 2 C, BeMgC and Mg 2 C using first-principles method
journal, January 2019


Lattice dynamics and elasticity in thermoelectric Mg 2 Si 1 x Sn x
journal, February 2019