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Title: Phonon anharmonicity and negative thermal expansion in SnSe

Authors:
; ; ; ; ; ; ;
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Solid-State Solar-Thermal Energy Conversion Center (S3TEC)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1388447
DOE Contract Number:
SC0001299; FG02-09ER46577
Resource Type:
Journal Article
Resource Relation:
Journal Name: Physical Review B; Journal Volume: 94; Journal Issue: 5; Related Information: S3TEC partners with Massachusetts Institute of Technology (lead); Boston College; Oak Ridge National Laboratory; Rensselaer Polytechnic Institute
Country of Publication:
United States
Language:
English
Subject:
solar (photovoltaic), solar (thermal), solid state lighting, phonons, thermal conductivity, thermoelectric, defects, mechanical behavior, charge transport, spin dynamics, materials and chemistry by design, optics, synthesis (novel materials), synthesis (self-assembly), synthesis (scalable processing)

Citation Formats

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., 2016. 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.
@article{osti_1388447,
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 = {},
doi = {10.1103/PhysRevB.94.054307},
journal = {Physical Review B},
number = 5,
volume = 94,
place = {United States},
year = 2016,
month = 8
}
  • Cited by 2
  • 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,more » 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.« less
  • 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 tomore » 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. Lastly, the origin of the anharmonic phonon thermodynamics is linked to the electronic structure.« less
  • Cubic scandium trifluoride (ScF{sub 3}) has a large negative thermal expansion over a wide range of temperatures. Inelastic neutron scattering experiments were performed to study the temperature dependence of the lattice dynamics of ScF{sub 3} from 7 to 750 K. The measured phonon densities of states show a large anharmonic contribution with a thermal stiffening of modes around 25 meV. Phonon calculations with first-principles methods identified the individual modes in the densities of states, and frozen phonon calculations showed that some of the modes with motions of F atoms transverse to their bond direction behave as quantum quartic oscillators. Themore » quartic potential originates from harmonic interatomic forces in the DO{sub 9} structure of ScF{sub 3}, and accounts for phonon stiffening with the temperature and a significant part of the negative thermal expansion.« less