Phonon anharmonicity and negative thermal expansion in SnSe
Abstract
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. Lastly, the origin of the anharmonic phonon thermodynamics is linked to the electronic structure.
- Authors:
-
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
- Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Quantum Condensed Matter Division
- 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:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF); Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1302905
- Alternate Identifier(s):
- OSTI ID: 1287766; OSTI ID: 1340000
- Grant/Contract Number:
- AC05-00OR22725; AC02-06CH11357; AC02-05CH11231; SC0001299; AC05- 00OR22725
- Resource 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)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 36 MATERIALS SCIENCE; phonon
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. https://doi.org/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. Tue .
"Phonon anharmonicity and negative thermal expansion in SnSe". United States. https://doi.org/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 = {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. Lastly, 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 = {Tue Aug 09 00:00:00 EDT 2016},
month = {Tue Aug 09 00:00:00 EDT 2016}
}
Web of Science
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
Phonon softening and metallization of a narrow-gap semiconductor by thermal disorder
journal, March 2011
- Delaire, O.; Marty, K.; Stone, M. B.
- Proceedings of the National Academy of Sciences, Vol. 108, Issue 12
Thermoelectric transport properties of pristine and Na-doped SnSe 1−x Te x polycrystals
journal, January 2015
- Wei, Tian-Ran; Wu, Chao-Feng; Zhang, Xiaozhi
- Physical Chemistry Chemical Physics, Vol. 17, Issue 44
Low thermal conductivity and triaxial phononic anisotropy of SnSe
journal, September 2014
- Carrete, Jesús; Mingo, Natalio; Curtarolo, Stefano
- Applied Physics Letters, Vol. 105, Issue 10
Generalized Grüneisen tensor from solid nonlinearity parameters
journal, May 1980
- Cantrell, John H.
- Physical Review B, Vol. 21, Issue 10
Complex thermoelectric materials
journal, February 2008
- Snyder, G. Jeffrey; Toberer, Eric S.
- Nature Materials, Vol. 7, Issue 2, p. 105-114
Resonant bonding leads to low lattice thermal conductivity
journal, April 2014
- Lee, Sangyeop; Esfarjani, Keivan; Luo, Tengfei
- Nature Communications, Vol. 5, Issue 1
The high temperature structure of β-SnS and β-SnSe and the B16-to-B33 type λ-transition path
journal, January 1981
- Schnering, Hans Georg von; Wiedemeier, Heribert
- Zeitschrift für Kristallographie - Crystalline Materials, Vol. 156, Issue 1-2
Record Seebeck coefficient and extremely low thermal conductivity in nanostructured SnSe
journal, February 2015
- Serrano-Sánchez, F.; Gharsallah, M.; Nemes, N. M.
- Applied Physics Letters, Vol. 106, Issue 8
Vibrational thermodynamics of materials
journal, May 2010
- Fultz, Brent
- Progress in Materials Science, Vol. 55, Issue 4
Electron-phonon coupling and thermal transport in the thermoelectric compound
journal, December 2015
- Bansal, Dipanshu; Li, Chen W.; Said, Ayman H.
- Physical Review B, Vol. 92, Issue 21
Ab initiomolecular dynamics for liquid metals
journal, January 1993
- Kresse, G.; Hafner, J.
- Physical Review B, Vol. 47, Issue 1, p. 558-561
High-efficient thermoelectric materials: The case of orthorhombic IV-VI compounds
journal, June 2015
- Ding, Guangqian; Gao, Guoying; Yao, Kailun
- Scientific Reports, Vol. 5, Article No. 9567
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
Neutron diffraction study of the structural phase transition in SnS and SnSe
journal, January 1986
- Chattopadhyay, T.; Pannetier, J.; Von Schnering, H. G.
- Journal of Physics and Chemistry of Solids, Vol. 47, Issue 9, p. 879-885
Microscopic mechanism of low thermal conductivity in lead telluride
journal, April 2012
- Shiga, Takuma; Shiomi, Junichiro; Ma, Jie
- Physical Review B, Vol. 85, Issue 15
Structural changes in thermoelectric SnSe at high pressures
journal, January 2015
- Loa, I.; Husband, R. J.; Downie, R. A.
- Journal of Physics: Condensed Matter, Vol. 27, Issue 7
Generalized Grüneisen Parameters in the Anisotropic Debye Model
journal, March 1965
- Brugger, K.
- Physical Review, Vol. 137, Issue 6A
Temperature and pressure induced phase transition in IV-VI compounds
journal, January 1984
- Chattopadhyay, T.; Werner, A.; von Schnering, H. G.
- Revue de Physique Appliquée, Vol. 19, Issue 9
Modeling non-harmonic behavior of materials from experimental inelastic neutron scattering and thermal expansion measurements
journal, July 2016
- Bansal, Dipanshu; Aref, Amjad; Dargush, Gary
- Journal of Physics: Condensed Matter, Vol. 28, Issue 38
The thermal expansion and high temperature transformation of SnS and SnSe*
journal, January 1979
- Wiedemeier, Heribert; Csillag, Frank J.
- Zeitschrift für Kristallographie - Crystalline Materials, Vol. 149, Issue 1-2
Giant anharmonic phonon scattering in PbTe
journal, June 2011
- Delaire, O.; Ma, J.; Marty, K.
- Nature Materials, Vol. 10, Issue 8, p. 614-619
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
Assessment of the thermoelectric performance of polycrystalline p-type SnSe
journal, May 2014
- Sassi, S.; Candolfi, C.; Vaney, J.-B.
- Applied Physics Letters, Vol. 104, Issue 21, Article No. 212105
A comparison of four direct geometry time-of-flight spectrometers at the Spallation Neutron Source
journal, April 2014
- Stone, M. B.; Niedziela, J. L.; Abernathy, D. L.
- Review of Scientific Instruments, Vol. 85, Issue 4
Bottom-up processing and low temperature transport properties of polycrystalline SnSe
journal, May 2015
- Ge, Zhen-Hua; Wei, Kaya; Lewis, Hutton
- Journal of Solid State Chemistry, Vol. 225
Phase diagram investigation and proposition of a thermodynamic evaluation of the Tin-Selenium system
journal, January 1996
- Feutelais, Y.; Majid, M.; Legendre, B.
- Journal of Phase Equilibria, Vol. 17, Issue 1
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
Peierls distortion as a route to high thermoelectric performance in In4Se3-δ crystals
journal, June 2009
- Rhyee, Jong-Soo; Lee, Kyu Hyoung; Lee, Sang Mock
- Nature, Vol. 459, Issue 7249
Orbitally driven giant phonon anharmonicity in SnSe
journal, October 2015
- Li, C. W.; Hong, J.; May, A. F.
- Nature Physics, Vol. 11, Issue 12
Thermoelectric performance of SnS and SnS–SnSe solid solution
journal, January 2015
- Han, Ye-Mao; Zhao, Jie; Zhou, Min
- Journal of Materials Chemistry A, Vol. 3, Issue 8
The mechanical and thermo-physical properties and electronic structures of SnS and SnSe in orthorhombic structure
journal, April 2013
- He, Xiancong; Shen, Honglie; Wang, Wei
- Journal of Alloys and Compounds, Vol. 556
Six-reflection meV-monochromator for synchrotron radiation
journal, May 2011
- Toellner, T. S.; Alatas, A.; Said, A. H.
- Journal of Synchrotron Radiation, Vol. 18, Issue 4
CONUSS and PHOENIX: Evaluation of nuclear resonant scattering data
journal, March 2000
- Sturhahn, W.
- Hyperfine Interactions, Vol. 125, Issue 1/4, p. 149-172
Capacité calorifique de l'alliage Sn0,50Se0,50 à l'état solide entre 375 et 1135 K
journal, July 1981
- Baldé, L.; Legendre, B.; Souleau, C.
- Journal of the Less Common Metals, Vol. 80, Issue 1
Electron-phonon interactions and high-temperature thermodynamics of vanadium and its alloys
journal, June 2008
- Delaire, O.; Kresch, M.; Muñoz, J. A.
- Physical Review B, Vol. 77, Issue 21
First-principles calculations of the ferroelastic transition between rutile-type and -type at high pressures
journal, October 2008
- Togo, Atsushi; Oba, Fumiyasu; Tanaka, Isao
- Physical Review B, Vol. 78, Issue 13
The Se−Sn (Selenium-Tin) system
journal, February 1986
- Sharma, R. C.; Chang, Y. A.
- Bulletin of Alloy Phase Diagrams, Vol. 7, Issue 1
Ultrahigh power factor and thermoelectric performance in hole-doped single-crystal SnSe
journal, November 2015
- Zhao, L.-D.; Tan, G.; Hao, S.
- Science, Vol. 351, Issue 6269, p. 141-144
Investigation of the Anisotropic Thermoelectric Properties of Oriented Polycrystalline SnSe
journal, June 2015
- Li, Yulong; Shi, Xun; Ren, Dudi
- Energies, Vol. 8, Issue 7
Structure and temperature transformation of SnSe. Stabilization of a new cubic phase Sn4Bi2Se7
journal, January 1998
- Adouby, K.; Pérez-Vicente, C.; Jumas, J. C.
- Zeitschrift für Kristallographie - Crystalline Materials, Vol. 213, Issue 6
Electronic structure and thermoelectric properties of - and -type SnSe from first-principles calculations
journal, May 2015
- Kutorasinski, K.; Wiendlocha, B.; Kaprzyk, S.
- Physical Review B, Vol. 91, Issue 20
Adiabatic Electron-Phonon Interaction and High-Temperature Thermodynamics of Compounds
journal, September 2008
- Delaire, O.; Lucas, M. S.; Muñoz, J. A.
- Physical Review Letters, Vol. 101, Issue 10
First-principles study of anisotropic thermoelectric transport properties of IV-VI semiconductor compounds SnSe and SnS
journal, September 2015
- Guo, Ruiqiang; Wang, Xinjiang; Kuang, Youdi
- Physical Review B, Vol. 92, Issue 11
Thermodynamics of Crystals
journal, November 1972
- Wallace, Duane C.; Callen, Herbert
- American Journal of Physics, Vol. 40, Issue 11
Complex thermoelectric materials
book, October 2010
- Snyder, G. Jeffrey; Toberer, Eric S.
- Materials for Sustainable Energy
High-resolution X-ray luminescence extension imaging
journal, February 2021
- Ou, Xiangyu; Qin, Xian; Huang, Bolong
- Nature, Vol. 590, Issue 7846
Microscopic mechanism of low thermal conductivity in lead-telluride
text, January 2012
- Shiga, Takuma; Shiomi, Junichiro; Ma, Jie
- arXiv
Low thermal conductivity and triaxial phononic anisotropy of SnSe
text, January 2014
- Carrete, Jesús; Mingo, Natalio; Curtarolo, Stefano
- arXiv
Structural Changes in Thermoelectric SnSe at High Pressures
text, January 2014
- Loa, I.; Husband, R. J.; Downie, R. A.
- arXiv
First-principles study of anisotropic thermoelectric transport properties of IV-VI semiconductor compounds SnSe and SnS
text, January 2015
- Guo, Ruiqiang; Wang, Xinjiang; Kuang, Youdi
- arXiv
Modeling non-harmonic behavior of materials from experimental inelastic neutron scattering and thermal expansion measurements
text, January 2016
- Bansal, Dipanshu; Aref, Amjad; Dargush, Gary
- arXiv
Works referencing / citing this record:
Phase Transformation Contributions to Heat Capacity and Impact on Thermal Diffusivity, Thermal Conductivity, and Thermoelectric Performance
journal, July 2019
- Agne, Matthias T.; Voorhees, Peter W.; Snyder, G. Jeffrey
- Advanced Materials, Vol. 31, Issue 35
Three-Stage Inter-Orthorhombic Evolution and High Thermoelectric Performance in Ag-Doped Nanolaminar SnSe Polycrystals
journal, June 2017
- Zhang, Lijuan; Wang, Jianli; Sun, Qiao
- Advanced Energy Materials, Vol. 7, Issue 19
High-Temperature Crystal Structure and Chemical Bonding in Thermoelectric Germanium Selenide (GeSe)
journal, April 2017
- Sist, Mattia; Gatti, Carlo; Nørby, Peter
- Chemistry - A European Journal, Vol. 23, Issue 28
Electronic and Thermoelectric Properties of SnSe1−xS x (x = 0, 0.25, 0.5, 0.75, and 1) Alloys: First-Principles Calculations
journal, April 2018
- Hamad, Bothina
- Journal of Electronic Materials, Vol. 47, Issue 7
Colossal barocaloric effects in plastic crystals
journal, March 2019
- Li, Bing; Kawakita, Yukinobu; Ohira-Kawamura, Seiko
- Nature, Vol. 567, Issue 7749
Enhancing thermoelectric performance by Fermi level tuning and thermal conductivity degradation in (Ge1−xBix)Te crystals
journal, June 2019
- Wei, Pai-Chun; Cai, Cheng-Xun; Hsing, Cheng-Rong
- Scientific Reports, Vol. 9, Issue 1
Anisotropic thermal expansion of SnSe from first-principles calculations based on Grüneisen's theory
journal, January 2017
- Liu, Gang; Zhou, Jian; Wang, Hui
- Physical Chemistry Chemical Physics, Vol. 19, Issue 23
Effects of temperature and pressure on the optical and vibrational properties of thermoelectric SnSe
journal, January 2019
- Efthimiopoulos, Ilias; Berg, Matthias; Bande, Annika
- Physical Chemistry Chemical Physics, Vol. 21, Issue 17
A practical field guide to thermoelectrics: Fundamentals, synthesis, and characterization
journal, June 2018
- Zevalkink, Alex; Smiadak, David M.; Blackburn, Jeff L.
- Applied Physics Reviews, Vol. 5, Issue 2
Phonon anharmonicity in thermoelectric palladium sulfide by Raman spectroscopy
journal, July 2018
- Chen, Liu-Cheng; Cao, Zi-Yu; Yu, Hao
- Applied Physics Letters, Vol. 113, Issue 2
Thermal expansion in insulating solids from first principles
journal, November 2019
- Ritz, Ethan T.; Li, Sabrina J.; Benedek, Nicole A.
- Journal of Applied Physics, Vol. 126, Issue 17
Lattice thermal conductivity of and SnSe using Debye-Callaway and Monte Carlo phonon transport modeling: Application to nanofilms and nanowires
journal, September 2019
- Al-Alam, Patricia; Pernot, Gilles; Isaiev, Mykola
- Physical Review B, Vol. 100, Issue 11
Investigation of the electronic structure and lattice dynamics of the thermoelectric material Na-doped SnSe
journal, September 2018
- Wu, P.; Zhang, B.; Peng, K. L.
- Physical Review B, Vol. 98, Issue 9
Critical mode and band-gap-controlled bipolar thermoelectric properties of SnSe
journal, August 2018
- Loa, I.; Popuri, S. R.; Fortes, A. D.
- Physical Review Materials, Vol. 2, Issue 8
Critical mode and band-gap-controlled bipolar thermoelectric properties of SnSe
text, January 2018
- Loa, I.; Popuri, S. R.; Fortes, A. D.
- arXiv
Colossal barocaloric effects in plastic crystals
text, January 2018
- Li, Bing; Kawakita, Yukinobu; Wang, Hui
- arXiv
Thermal Expansion in Insulating Solids From First Principles
text, January 2019
- Ritz, Ethan T.; Li, Sabrina J.; Benedek, Nicole A.
- arXiv