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Title: 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:
ORCiD logo [1];  [2];  [2]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [5]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1];  [2]
+ Show Author Affiliations
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
  2. California Inst. of Technology (CalTech), Pasadena, CA (United States). Division of Engineering and Applied Science
  3. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States). Center for Neutron Research
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Scattering Division
  5. 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) (SC-22); 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.
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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. doi:10.1038/s41467-019-09921-4.
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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. doi:10.1038/s41467-019-09921-4. https://www.osti.gov/servlets/purl/1511918.
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@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}
}
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DOI:  10.1038/s41467-019-09921-4
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Works referenced in this record:

Projector augmented-wave method
journal, December 1994

Complex thermoelectric materials
journal, February 2008

  • Snyder, G. Jeffrey; Toberer, Eric S.
  • Nature Materials, Vol. 7, Issue 2, p. 105-114
  • DOI: 10.1038/nmat2090

New Directions for Low-Dimensional Thermoelectric Materials
journal, April 2007

  • Dresselhaus, M.?S.; Chen, G.; Tang, M.?Y.
  • Advanced Materials, Vol. 19, Issue 8, p. 1043-1053
  • DOI: 10.1002/adma.200600527

From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999

Convergence of electronic bands for high performance bulk thermoelectrics
journal, May 2011

  • Pei, Yanzhong; Shi, Xiaoya; LaLonde, Aaron
  • Nature, Vol. 473, Issue 7345, p. 66-69
  • DOI: 10.1038/nature09996

High-performance bulk thermoelectrics with all-scale hierarchical architectures
journal, September 2012

  • Biswas, Kanishka; He, Jiaqing; Blum, Ivan D.
  • Nature, Vol. 489, Issue 7416, p. 414-418
  • DOI: 10.1038/nature11439

Giant anharmonic phonon scattering in PbTe
journal, June 2011

  • Delaire, O.; Ma, J.; Marty, K.
  • Nature Materials, Vol. 10, Issue 8, p. 614-619
  • DOI: 10.1038/nmat3035

Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996

Materials for thermoelectric energy conversion
journal, April 1988

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996

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