Orbitally driven giant phonon anharmonicity in SnSe

C. W. Li; J. Hong; A. F. May; D. Bansal; S. Chi; T. Hong; G. Ehlers; O. Delaire

doi:10.1038/nphys3492

Orbitally driven giant phonon anharmonicity in SnSe

C. W. Li, J. Hong, A. F. May, D. Bansal, S. Chi, T. Hong, G. Ehlers, O. Delaire

Research output: Contribution to journal › Article › peer-review

585 Scopus citations

Abstract

Understanding elementary excitations and their couplings in condensed matter systems is critical for developing better energy-conversion devices. In thermoelectric materials, the heat-to-electricity conversion efficiency is directly improved by suppressing the propagation of phonon quasiparticles responsible for macroscopic thermal transport. The current record material for thermoelectric conversion efficiency, SnSe, has an ultralow thermal conductivity, but the mechanism behind the strong phonon scattering remains largely unknown. From inelastic neutron scattering measurements and first-principles simulations, we mapped the four-dimensional phonon dispersion surfaces of SnSe, and found the origin of the ionic-potential anharmonicity responsible for the unique properties of SnSe. We show that the giant phonon scattering arises from an unstable electronic structure, with orbital interactions leading to a ferroelectric-like lattice instability. The present results provide a microscopic picture connecting electronic structure and phonon anharmonicity in SnSe, and offers new insights on how electron-phonon and phonon-phonon interactions may lead to the realization of ultralow thermal conductivity.

Original language	English
Pages (from-to)	1063-1069
Number of pages	7
Journal	Nature Physics
Volume	11
Issue number	12
DOIs	https://doi.org/10.1038/nphys3492
State	Published - Dec 1 2015

Funding

Neutron scattering measurements and analysis (O.D., C.W.L.) was supported as part of the S3TEC EFRC, an Energy Frontier Research Center funded by the US Department of Energy, Office of Science, Basic Energy Sciences under Award # DE-SC0001299. Computer simulations and analysis were supported through CAMM (J.H., D.B.), funded by the US Department of Energy, Basic Energy Sciences, Materials Sciences and Engineering Division. Sample synthesis (A.F.M.) was supported by the US Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. The use of Oak Ridge National Laboratory’s Spallation Neutron Source and High Flux Isotope Reactor was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, US Department of Energy. The orientation of single crystals was characterized using the X-ray Laue camera system at the X-ray lab in SNS, ORNL (we thank J. K. Keum for his assistance). This research used resources of the Oak Ridge Leadership Computing Facility (OLCF), which is supported by the Office of Science of the US Department of Energy.

Funders	Funder number
CAMM
Office of Basic Energy Sciences
S3TEC EFRC
Scientific User Facilities Division
US Department of Energy
Office of Science
Basic Energy Sciences	DE-SC0001299
Oak Ridge National Laboratory
Division of Materials Sciences and Engineering

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AU - May, A. F.

AU - Bansal, D.

AU - Chi, S.

AU - Hong, T.

AU - Ehlers, G.

AU - Delaire, O.

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AB - Understanding elementary excitations and their couplings in condensed matter systems is critical for developing better energy-conversion devices. In thermoelectric materials, the heat-to-electricity conversion efficiency is directly improved by suppressing the propagation of phonon quasiparticles responsible for macroscopic thermal transport. The current record material for thermoelectric conversion efficiency, SnSe, has an ultralow thermal conductivity, but the mechanism behind the strong phonon scattering remains largely unknown. From inelastic neutron scattering measurements and first-principles simulations, we mapped the four-dimensional phonon dispersion surfaces of SnSe, and found the origin of the ionic-potential anharmonicity responsible for the unique properties of SnSe. We show that the giant phonon scattering arises from an unstable electronic structure, with orbital interactions leading to a ferroelectric-like lattice instability. The present results provide a microscopic picture connecting electronic structure and phonon anharmonicity in SnSe, and offers new insights on how electron-phonon and phonon-phonon interactions may lead to the realization of ultralow thermal conductivity.

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Orbitally driven giant phonon anharmonicity in SnSe

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