Extended anharmonic collapse of phonon dispersions in SnS and SnSe
Abstract
The lattice dynamics and high-temperature structural transition in SnS and SnSe are investigated via inelastic neutron scattering, high-resolution Raman spectroscopy and anharmonic first-principles simulations. We uncover a spectacular, extreme softening and reconstruction of an entire manifold of low-energy acoustic and optic branches across a structural transition, reflecting strong directionality in bonding strength and anharmonicity. Further, our results solve a prior controversy by revealing the soft-mode mechanism of the phase transition that impacts thermal transport and thermoelectric efficiency. Our simulations of anharmonic phonon renormalization go beyond low-order perturbation theory and capture these striking effects, showing that the large phonon shifts directly affect the thermal conductivity by altering both the phonon scattering phase space and the group velocities. These results provide a detailed microscopic understanding of phase stability and thermal transport in technologically important materials, providing further insights on ways to control phonon propagation in thermoelectrics, photovoltaics, and other materials requiring thermal management.
- Authors:
-
[1];
[2];
[2];
[3];
[2];
[2];
[2];
[2];
[2];
[1]
- Duke Univ., Durham, NC (United States)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS), High Flux Isotope Reactor (HFIR), and Center for Nanophase Materials Science (CNMS); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Duke Univ., Durham, NC (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division
- OSTI Identifier:
- 1659620
- Alternate Identifier(s):
- OSTI ID: 1660759
- Grant/Contract Number:
- AC05-00OR22725; SC0019299; SC0016166; AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 11; Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; Phase transitions and critical phenomena; Thermoelectrics; thermoelectrics, lattice dynamics, phonons, anharmonicity, thermal transport, phase transitions
Citation Formats
Lanigan-Atkins, Tyson, Yang, S., Niedziela, Jennifer L., Bansal, Dipanshu, May, Andrew F., Puretzky, Alexander A., Lin, Jiao Y., Pajerowski, Daniel M., Hong, Tao, Chi, Songxue, Ehlers, Georg, and Delaire, O. Extended anharmonic collapse of phonon dispersions in SnS and SnSe. United States: N. p., 2020.
Web. doi:10.1038/s41467-020-18121-4.
Lanigan-Atkins, Tyson, Yang, S., Niedziela, Jennifer L., Bansal, Dipanshu, May, Andrew F., Puretzky, Alexander A., Lin, Jiao Y., Pajerowski, Daniel M., Hong, Tao, Chi, Songxue, Ehlers, Georg, & Delaire, O. Extended anharmonic collapse of phonon dispersions in SnS and SnSe. United States. https://doi.org/10.1038/s41467-020-18121-4
Lanigan-Atkins, Tyson, Yang, S., Niedziela, Jennifer L., Bansal, Dipanshu, May, Andrew F., Puretzky, Alexander A., Lin, Jiao Y., Pajerowski, Daniel M., Hong, Tao, Chi, Songxue, Ehlers, Georg, and Delaire, O. Fri .
"Extended anharmonic collapse of phonon dispersions in SnS and SnSe". United States. https://doi.org/10.1038/s41467-020-18121-4. https://www.osti.gov/servlets/purl/1659620.
@article{osti_1659620,
title = {Extended anharmonic collapse of phonon dispersions in SnS and SnSe},
author = {Lanigan-Atkins, Tyson and Yang, S. and Niedziela, Jennifer L. and Bansal, Dipanshu and May, Andrew F. and Puretzky, Alexander A. and Lin, Jiao Y. and Pajerowski, Daniel M. and Hong, Tao and Chi, Songxue and Ehlers, Georg and Delaire, O.},
abstractNote = {The lattice dynamics and high-temperature structural transition in SnS and SnSe are investigated via inelastic neutron scattering, high-resolution Raman spectroscopy and anharmonic first-principles simulations. We uncover a spectacular, extreme softening and reconstruction of an entire manifold of low-energy acoustic and optic branches across a structural transition, reflecting strong directionality in bonding strength and anharmonicity. Further, our results solve a prior controversy by revealing the soft-mode mechanism of the phase transition that impacts thermal transport and thermoelectric efficiency. Our simulations of anharmonic phonon renormalization go beyond low-order perturbation theory and capture these striking effects, showing that the large phonon shifts directly affect the thermal conductivity by altering both the phonon scattering phase space and the group velocities. These results provide a detailed microscopic understanding of phase stability and thermal transport in technologically important materials, providing further insights on ways to control phonon propagation in thermoelectrics, photovoltaics, and other materials requiring thermal management.},
doi = {10.1038/s41467-020-18121-4},
journal = {Nature Communications},
number = 1,
volume = 11,
place = {United States},
year = {Fri Sep 04 00:00:00 EDT 2020},
month = {Fri Sep 04 00:00:00 EDT 2020}
}
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