Intrinsic anharmonic localization in thermoelectric PbSe
Abstract
Lead chalcogenides have exceptional thermoelectric properties and intriguing anharmonic lattice dynamics underlying their low thermal conductivities. An ideal material for thermoelectric efficiency is the phonon glass-electron crystal, which drives research on strategies to scatter or localize phonons while minimally disrupting electronic-transport. Anharmonicity can potentially do both, even in perfect crystals, and simulations suggest that PbSe is anharmonic enough to support intrinsic localized modes that halt transport. Here, we experimentally observe high-temperature localization in PbSe using neutron scattering but find that localization is not limited to isolated modes - zero group velocity develops for a significant section of the transverse optic phonon on heating above a transition in the anharmonic dynamics. Arrest of the optic phonon propagation coincides with unusual sharpening of the longitudinal acoustic mode due to a loss of phase space for scattering. Our study shows how nonlinear physics beyond conventional anharmonic perturbations can fundamentally alter vibrational transport properties.
- Authors:
-
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
- California Inst. of Technology (CalTech), Pasadena, CA (United States). Division of Engineering and Applied Science
- National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States). Center for Neutron Research
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Scattering Division
- Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
- Publication Date:
- Research Org.:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); Defense Advanced Research Projects Agency (DARPA); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; National Institute of Standards and Technology (NIST); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); U.S. Department of Defense (DOD), Defense Advanced Research Projects Agency (DARPA)
- OSTI Identifier:
- 1511918
- Alternate Identifier(s):
- OSTI ID: 1512254
- Grant/Contract Number:
- AC05-00OR22725; AC02-06CH11357; HR0011-15-2-0039
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Manley, Michael E., Hellman, O., Shulumba, Nina, May, Andrew F., Stonaha, Paul J., Lynn, Jeffrey, Garlea, Vasile O., Alatas, Ahmet, Hermann, Raphael P., Budai, John D., Wang, Hsin, Sales, Brian C., and Minnich, Austin. Intrinsic anharmonic localization in thermoelectric PbSe. United States: N. p., 2019.
Web. doi:10.1038/s41467-019-09921-4.
Manley, Michael E., Hellman, O., Shulumba, Nina, May, Andrew F., Stonaha, Paul J., Lynn, Jeffrey, Garlea, Vasile O., Alatas, Ahmet, Hermann, Raphael P., Budai, John D., Wang, Hsin, Sales, Brian C., & Minnich, Austin. Intrinsic anharmonic localization in thermoelectric PbSe. United States. https://doi.org/10.1038/s41467-019-09921-4
Manley, Michael E., Hellman, O., Shulumba, Nina, May, Andrew F., Stonaha, Paul J., Lynn, Jeffrey, Garlea, Vasile O., Alatas, Ahmet, Hermann, Raphael P., Budai, John D., Wang, Hsin, Sales, Brian C., and Minnich, Austin. Fri .
"Intrinsic anharmonic localization in thermoelectric PbSe". United States. https://doi.org/10.1038/s41467-019-09921-4. https://www.osti.gov/servlets/purl/1511918.
@article{osti_1511918,
title = {Intrinsic anharmonic localization in thermoelectric PbSe},
author = {Manley, Michael E. and Hellman, O. and Shulumba, Nina and May, Andrew F. and Stonaha, Paul J. and Lynn, Jeffrey and Garlea, Vasile O. and Alatas, Ahmet and Hermann, Raphael P. and Budai, John D. and Wang, Hsin and Sales, Brian C. and Minnich, Austin},
abstractNote = {Lead chalcogenides have exceptional thermoelectric properties and intriguing anharmonic lattice dynamics underlying their low thermal conductivities. An ideal material for thermoelectric efficiency is the phonon glass-electron crystal, which drives research on strategies to scatter or localize phonons while minimally disrupting electronic-transport. Anharmonicity can potentially do both, even in perfect crystals, and simulations suggest that PbSe is anharmonic enough to support intrinsic localized modes that halt transport. Here, we experimentally observe high-temperature localization in PbSe using neutron scattering but find that localization is not limited to isolated modes - zero group velocity develops for a significant section of the transverse optic phonon on heating above a transition in the anharmonic dynamics. Arrest of the optic phonon propagation coincides with unusual sharpening of the longitudinal acoustic mode due to a loss of phase space for scattering. Our study shows how nonlinear physics beyond conventional anharmonic perturbations can fundamentally alter vibrational transport properties.},
doi = {10.1038/s41467-019-09921-4},
journal = {Nature Communications},
number = 1,
volume = 10,
place = {United States},
year = {2019},
month = {4}
}
Web of Science
Figures / Tables:

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Figures / Tables found in this record: