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Title: Phonon anharmonicity and negative thermal expansion in SnSe

In this paper, the anharmonic phonon properties of SnSe in the Pnma phase were investigated with a combination of experiments and first-principles simulations. Using inelastic neutron scattering (INS) and nuclear resonant inelastic X-ray scattering (NRIXS), we have measured the phonon dispersions and density of states (DOS) and their temperature dependence, which revealed a strong, inhomogeneous shift and broadening of the spectrum on warming. First-principles simulations were performed to rationalize these measurements, and to explain the previously reported anisotropic thermal expansion, in particular the negative thermal expansion within the Sn-Se bilayers. Including the anisotropic strain dependence of the phonon free energy, in addition to the electronic ground state energy, is essential to reproduce the negative thermal expansion. From the phonon DOS obtained with INS and additional calorimetry measurements, we quantify the harmonic, dilational, and anharmonic components of the phonon entropy, heat capacity, and free energy. Finally, the origin of the anharmonic phonon thermodynamics is linked to the electronic structure.
Authors:
 [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [2] ;  [3] ;  [4]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Quantum Condensed Matter Division
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division; Duke Univ., Durham, NC (United States). Mechanical Engineering and Materials Science Dept.
Publication Date:
Grant/Contract Number:
AC05-00OR22725; AC02-06CH11357; AC02-05CH11231; SC0001299; AC05- 00OR22725
Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 94; Journal Issue: 5; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF); Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 36 MATERIALS SCIENCE; phonon
OSTI Identifier:
1302905
Alternate Identifier(s):
OSTI ID: 1287766; OSTI ID: 1340000

Bansal, Dipanshu, Hong, Jiawang, Li, Chen W., May, Andrew F., Porter, Wallace, Hu, Michael Y., Abernathy, Douglas L., and Delaire, Olivier. Phonon anharmonicity and negative thermal expansion in SnSe. United States: N. p., Web. doi:10.1103/PhysRevB.94.054307.
Bansal, Dipanshu, Hong, Jiawang, Li, Chen W., May, Andrew F., Porter, Wallace, Hu, Michael Y., Abernathy, Douglas L., & Delaire, Olivier. Phonon anharmonicity and negative thermal expansion in SnSe. United States. doi:10.1103/PhysRevB.94.054307.
Bansal, Dipanshu, Hong, Jiawang, Li, Chen W., May, Andrew F., Porter, Wallace, Hu, Michael Y., Abernathy, Douglas L., and Delaire, Olivier. 2016. "Phonon anharmonicity and negative thermal expansion in SnSe". United States. doi:10.1103/PhysRevB.94.054307. https://www.osti.gov/servlets/purl/1302905.
@article{osti_1302905,
title = {Phonon anharmonicity and negative thermal expansion in SnSe},
author = {Bansal, Dipanshu and Hong, Jiawang and Li, Chen W. and May, Andrew F. and Porter, Wallace and Hu, Michael Y. and Abernathy, Douglas L. and Delaire, Olivier},
abstractNote = {In this paper, the anharmonic phonon properties of SnSe in the Pnma phase were investigated with a combination of experiments and first-principles simulations. Using inelastic neutron scattering (INS) and nuclear resonant inelastic X-ray scattering (NRIXS), we have measured the phonon dispersions and density of states (DOS) and their temperature dependence, which revealed a strong, inhomogeneous shift and broadening of the spectrum on warming. First-principles simulations were performed to rationalize these measurements, and to explain the previously reported anisotropic thermal expansion, in particular the negative thermal expansion within the Sn-Se bilayers. Including the anisotropic strain dependence of the phonon free energy, in addition to the electronic ground state energy, is essential to reproduce the negative thermal expansion. From the phonon DOS obtained with INS and additional calorimetry measurements, we quantify the harmonic, dilational, and anharmonic components of the phonon entropy, heat capacity, and free energy. Finally, the origin of the anharmonic phonon thermodynamics is linked to the electronic structure.},
doi = {10.1103/PhysRevB.94.054307},
journal = {Physical Review B},
number = 5,
volume = 94,
place = {United States},
year = {2016},
month = {8}
}

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

Complex thermoelectric materials
journal, February 2008
  • Snyder, G. Jeffrey; Toberer, Eric S.
  • Nature Materials, Vol. 7, Issue 2, p. 105-114
  • DOI: 10.1038/nmat2090

Ab initiomolecular dynamics for liquid metals
journal, January 1993

Ultralow thermal conductivity and high thermoelectric figure of merit in SnSe crystals
journal, April 2014
  • Zhao, Li-Dong; Lo, Shih-Han; Zhang, Yongsheng
  • Nature, Vol. 508, Issue 7496, p. 373-377
  • DOI: 10.1038/nature13184

Giant anharmonic phonon scattering in PbTe
journal, June 2011
  • Delaire, O.; Ma, J.; Marty, K.
  • Nature Materials, Vol. 10, Issue 8, p. 614-619
  • DOI: 10.1038/nmat3035

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

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