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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]
  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); 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. 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., 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.
@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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Cited by: 5 works
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Figures / Tables:

Fig. 1 Fig. 1: Triple-axis thermal neutron scattering measurements of the phonons PbSe. a Summary of the temperature dependence of the measured phonon dispersion for the transverse acoustic (TA), longitudinal acoustic (LA), and transverse optic (TO) phonons folded into the first zone along phonon wavevector q = [h, h, 0]. The datamore » points were determined by fitting Lorentzians to the data. The flattening of the TO phonon at 793 K indicates a phonon group velocity, v$g$ = d$E$/d$q$, that goes to zero (localization). b–d Temperature dependence of the spectral intensity distribution for the TO phonon measured in the (113) zone along scattering wavevector Q = [H, H, 3]. Data sets are offset for clarity. e, f Temperature dependence of the spectral intensity distribution for the LA and TA phonons. The TA appears despite the longitudinal geometry because of finite Q resolution effects. Surprisingly, the LA phonon is sharper at 793 K than at 643 K. Intensity bars are in counts. Error bars are statistical and represent one s.d.« less

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