Anharmonic properties in 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:
-
- 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}
}
Web of Science
Works referenced in this record:
Density-Functional Perturbation Theory for Quasi-Harmonic Calculations
journal, January 2010
- Baroni, S.; Giannozzi, P.; Isaev, E.
- Reviews in Mineralogy and Geochemistry, Vol. 71, Issue 1
Anharmonic effects in Mg2X (X = Si, Ge, Sn) compounds studied by Raman spectroscopy
journal, January 1987
- Raptis, Y. S.; Kourouklis, G. A.; Anastassakis, E.
- Journal de Physique, Vol. 48, Issue 2
Ab initio thermal transport in compound semiconductors
journal, April 2013
- Lindsay, L.; Broido, D. A.; Reinecke, T. L.
- Physical Review B, Vol. 87, Issue 16
Lattice thermal conductivity of MgO at conditions of Earth's interior
journal, February 2010
- Tang, X.; Dong, J.
- Proceedings of the National Academy of Sciences, Vol. 107, Issue 10
Projector augmented-wave method
journal, December 1994
- Blöchl, P. E.
- Physical Review B, Vol. 50, Issue 24, p. 17953-17979
Lattice Dynamics of Pb at Room Temperature
journal, March 1972
- Wakabayashi, N.; Ahmad, A. A. Z.; Shanks, H. R.
- Physical Review B, Vol. 5, Issue 6
Highly effective thermoelectrics
journal, July 2006
- Zaitsev, V. K.; Fedorov, M. I.; Gurieva, E. A.
- Physical Review B, Vol. 74, Issue 4
Phonon-Mediated Thermal Conductivity in Ionic Solids by Lattice Dynamics-Based Methods
journal, July 2011
- Chernatynskiy, Aleksandr; Turney, Joseph E.; McGaughey, Alan J. H.
- Journal of the American Ceramic Society, Vol. 94, Issue 10
Elastic constants and calculated lattice vibration frequencies of Mg2Sn
journal, March 1967
- Davis, L. C.; Whitten, W. B.; Danielson, G. C.
- Journal of Physics and Chemistry of Solids, Vol. 28, Issue 3
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
Lattice dynamics of magnesium stannide at room temperature
journal, May 1970
- Kearney, R. J.; Worlton, T. G.; Schmunk, R. E.
- Journal of Physics and Chemistry of Solids, Vol. 31, Issue 5
Bonding in Mg2Si Studied with X-ray Photoelectron Spectroscopy
journal, June 1995
- van Buuren, M. R. J.; Voermans, F.; vanKempen, H.
- The Journal of Physical Chemistry, Vol. 99, Issue 23
Bipolar Electronic Thermal Conductivity in Semimetals
journal, October 1962
- Gallo, C. F.; Miller, R. C.; Sutter, P. H.
- Journal of Applied Physics, Vol. 33, Issue 10
Lattice dynamics of Mg2Ge
journal, December 1965
- Chung, P. L.; Whitten, W. B.; Danielson, G. C.
- Journal of Physics and Chemistry of Solids, Vol. 26, Issue 12
Melt growth and characterization of Mg2Si bulk crystals
journal, August 2007
- Tamura, Daiki; Nagai, Ryo; Sugimoto, Kazuhiro
- Thin Solid Films, Vol. 515, Issue 22
In situ X-ray observation of phase transitions in under high pressure
journal, May 2009
- Hao, Jian; Zou, Bo; Zhu, Pinwen
- Solid State Communications, Vol. 149, Issue 17-18
Synthesis of Mg 2 C: A Magnesium Methanide
journal, July 2013
- Kurakevych, Oleksandr O.; Strobel, Timothy A.; Kim, Duck Young
- Angewandte Chemie International Edition, Vol. 52, Issue 34
Phonon Lifetime Investigation of Anharmonicity and Thermal Conductivity of by Neutron Scattering and Theory
journal, April 2013
- Pang, Judy W. L.; Buyers, William J. L.; Chernatynskiy, Aleksandr
- Physical Review Letters, Vol. 110, Issue 15
Evaluation of computational techniques for solving the Boltzmann transport equation for lattice thermal conductivity calculations
journal, October 2010
- Chernatynskiy, Aleksandr; Phillpot, Simon R.
- Physical Review B, Vol. 82, Issue 13
Vibrational thermodynamics of materials
journal, May 2010
- Fultz, Brent
- Progress in Materials Science, Vol. 55, Issue 4
Ab initiomolecular dynamics for liquid metals
journal, January 1993
- Kresse, G.; Hafner, J.
- Physical Review B, Vol. 47, Issue 1, p. 558-561
First-principles studies of intrinsic point defects in magnesium silicide
journal, April 2009
- Kato, Akihiko; Yagi, Takeshi; Fukusako, Naoto
- Journal of Physics: Condensed Matter, Vol. 21, Issue 20
Neutron scattering investigation of lattice dynamics and thermally induced disorder in the antifluorite Mg2Si
journal, September 1988
- Hutchings, M.
- Solid State Ionics, Vol. 28-30
Phonon conduction in PbSe, PbTe, and PbTe Se from first-principles calculations
journal, May 2012
- Tian, Zhiting; Garg, Jivtesh; Esfarjani, Keivan
- Physical Review B, Vol. 85, Issue 18
Ab initio theory of the lattice thermal conductivity in diamond
journal, September 2009
- Ward, A.; Broido, D. A.; Stewart, Derek A.
- Physical Review B, Vol. 80, Issue 12
Phonon Transport Simulator (PhonTS)
journal, July 2015
- Chernatynskiy, Aleksandr; Phillpot, Simon R.
- Computer Physics Communications, Vol. 192
First-principles investigation of the electronic and lattice vibrational properties of Mg 2 C
journal, October 2014
- Li, Tongwei; Ju, Weiwei; Liu, Huihui
- Computational Materials Science, Vol. 93
Thermal conductivity of argon at high pressure from first principles calculations
journal, August 2013
- Chernatynskiy, Aleksandr; Phillpot, Simon R.
- Journal of Applied Physics, Vol. 114, Issue 6
Direct Solution to the Linearized Phonon Boltzmann Equation
journal, June 2013
- Chaput, Laurent
- Physical Review Letters, Vol. 110, Issue 26
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
Thermal stability and elastic properties of Mg2X (X=Si, Ge, Sn, Pb) phases from first-principle calculations
journal, January 2012
- Zhou, Dianwu; Liu, Jinshui; Xu, Shaohua
- Computational Materials Science, Vol. 51, Issue 1
Raman Scattering in Si, Ge, and Sn
journal, April 1971
- Buchenauer, C. J.; Cardona, M.
- Physical Review B, Vol. 3, Issue 8
Studies on AB2-type intermetallic compounds, I. Mg2Ge and Mg2Sn: single-crystal structure refinement and ab initio calculations
journal, March 1996
- Grosch, Georg H.; Range, Klaus-Jürgen
- Journal of Alloys and Compounds, Vol. 235, Issue 2
Thermoelectric Performance of Sb- and La-Doped Mg2Si0.5Ge0.5
journal, March 2012
- Zhou, Xiaoyuan; Wang, Guoyu; Chi, Hang
- Journal of Electronic Materials, Vol. 41, Issue 6
Lattice dynamics in intermetallic Mg 2 Ge and Mg 2 Si
journal, November 2014
- Bessas, D.; Simon, R. E.; Friese, K.
- Journal of Physics: Condensed Matter, Vol. 26, Issue 48
Mechanochemical synthesis and thermoelectric properties of high quality magnesium silicide
journal, January 2011
- Bux, Sabah K.; Yeung, Michael T.; Toberer, Eric S.
- Journal of Materials Chemistry, Vol. 21, Issue 33
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
Thermodynamic properties of Mg2Si and Mg2Ge investigated by first principles method
journal, June 2010
- Wang, Hanfu; Jin, Hao; Chu, Weiguo
- Journal of Alloys and Compounds, Vol. 499, Issue 1
Simple view of the phonon spectrum: Sn resonances and mean field
journal, February 2015
- Chaput, Laurent; Bourgeois, Julie; Prytuliak, Anastasiia
- Physical Review B, Vol. 91, Issue 6
Ab initio molecular-dynamics simulation of the liquid-metal–amorphous-semiconductor transition in germanium
journal, May 1994
- Kresse, G.; Hafner, J.
- Physical Review B, Vol. 49, Issue 20, p. 14251-14269
Thermal study of group II–IV semiconductors—I. Heat capacity of Mg2Ge in the range 5–300°K
journal, June 1966
- Gerstein, B. C.; Chung, P. L.; Danielson, G. C.
- Journal of Physics and Chemistry of Solids, Vol. 27, Issue 6-7
Thermal conductivity of bulk and nanowire Mg Si Sn alloys from first principles
journal, November 2012
- Li, Wu; Lindsay, L.; Broido, D. A.
- Physical Review B, Vol. 86, Issue 17
Debye temperatures of 24 cubic elements by three methods
journal, October 1969
- Konti, A.; Varshni, Y. P.
- Canadian Journal of Physics, Vol. 47, Issue 19
Thermal conductivity of magnesium plumbide
journal, June 1974
- Martin, J. J.; Shanks, H. R.
- Journal of Applied Physics, Vol. 45, Issue 6
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
- Gerstein, B. C.; Jelinek, F. J.; Habenschuss, M.
- The Journal of Chemical Physics, Vol. 47, Issue 6
Isotope scattering of large-wave-vector phonons in GaAs and InSb: Deformation-dipole and overlap-shell models
journal, July 1984
- Tamura, Shin-ichiro
- Physical Review B, Vol. 30, Issue 2
Infrared Reflectivities of Magnesium Silicide, Germanide, and Stannide
journal, June 1963
- McWilliams, D.; Lynch, D. W.
- Physical Review, Vol. 130, Issue 6
Lattice dynamics of Mg2Si and Mg2Ge compounds from first-principles calculations
journal, May 2008
- Tani, Jun-ichi; Kido, Hiroyasu
- Computational Materials Science, Vol. 42, Issue 3
Effective charge on silicon atom in the metal silicides and CaSi
journal, May 2005
- Ishii, Hideshi; Matsuo, Shuji; Karimov, Pavel
- Physical Review B, Vol. 71, Issue 20
Magnetron Deposition of In Situ Thermoelectric Mg2Ge Thin Films
journal, February 2009
- Chuang, L.; Savvides, N.; Li, S.
- Journal of Electronic Materials, Vol. 38, Issue 7
Thermal study of II–IV semiconductors: Heat capacity and thermodynamic functions of Mg2Pb from 5–300°K
journal, November 1971
- Schwartz, R. G.; Shanks, H.; Gerstein, B. C.
- Journal of Solid State Chemistry, Vol. 3, Issue 4
Defect and phase stability of solid solutions of Mg2X with an antifluorite structure: An ab initio study
journal, September 2012
- Viennois, Romain; Jund, Philippe; Colinet, Catherine
- Journal of Solid State Chemistry, Vol. 193
X-Ray characteristic temperature and thermal expansion coefficient of Mg2Ge
journal, November 1973
- Dutchak, I. Ya.; Yarmolyuk, V. P.
- Soviet Physics Journal, Vol. 16, Issue 11
Lattice dynamics of magnesium stannide at room temperature
journal, December 1969
- Kearney, R. J.; Worlton, T. G.; Schmunk, R. E.
- Solid State Communications, Vol. 7, Issue 24
Reducing Dzyaloshinskii-Moriya interaction and field-free spin-orbit torque switching in synthetic antiferromagnets
journal, May 2021
- Chen, Ruyi; Cui, Qirui; Liao, Liyang
- Nature Communications, Vol. 12, Issue 1
High-resolution X-ray luminescence extension imaging
journal, February 2021
- Ou, Xiangyu; Qin, Xian; Huang, Bolong
- Nature, Vol. 590, Issue 7846
Electronic structure of AlFeN films exhibiting crystallographic orientation change from c- to a-axis with Fe concentrations and annealing effect
journal, February 2020
- Tatemizo, Nobuyuki; Imada, Saki; Okahara, Kizuna
- Scientific Reports, Vol. 10, Issue 1
Synthesis of Mg 2 C: A Magnesium Methanide
journal, July 2013
- Kurakevych, Oleksandr O.; Strobel, Timothy A.; Kim, Duck Young
- Angewandte Chemie, Vol. 125, Issue 34
Elastic constants and calculated lattice vibration frequencies of Mg2Sn
journal, November 1966
- Davis, L. C.; Whitten, W. B.; Danielson, G. C.
- Solid State Communications, Vol. 4, Issue 11
Ab initio theory of the lattice thermal conductivity in diamond
text, January 2009
- Ward, Alister; Broido, David; Stewart, Derek A.
- Universität Regensburg
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
- Maurya, V.; Paliwal, U.; Sharma, G.
- RSC Advances, Vol. 9, Issue 24
Lattice dynamics and elasticity in thermoelectric
journal, February 2019
- Klobes, Benedikt; de Boor, Johannes; Alatas, Ahmet
- Physical Review Materials, Vol. 3, Issue 2