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.
| Original language | English |
|---|---|
| Article number | 1928 |
| Journal | Nature Communications |
| Volume | 10 |
| Issue number | 1 |
| DOIs | |
| State | Published - Dec 1 2019 |
Funding
The authors thank D. Bansal for assistance in orienting the PbSe crystal. This work was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division under Contract Number DE-AC05-00OR22725. A portion of this research performed at the Oak Ridge National Laboratory’s Spallation Neutron Source was sponsored by the US Department of Energy, Office of Basic Energy Sciences. The authors acknowledge the support of the National Institute of Standards and Technology, US Department of Commerce, in providing the neutron research facilities used in this work. The identification of any commercial product or trade name does not imply endorsement or recommendation by the National Institute of Standards and Technology. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. H. Wang’s effort was sponsored by the DOE Energy Efficiency and Renewable Energy, Office of Vehicle Technologies Materials program. N.S. and A.J.M. acknowledge the support of the DARPA MATRIX program under Grant No. HR0011-15-2-0039. This work used the Extreme Science and Engineering Discovery Environment (XSEDE), which is supported by National Science Foundation Grant No. ACI-1053575.
| Funders | Funder number |
|---|---|
| DOE Office of Science | |
| Office of Basic Energy Sciences | |
| US Department of Energy | |
| National Science Foundation | |
| U.S. Department of Energy | |
| Directorate for Computer and Information Science and Engineering | 1053575 |
| National Institute of Standards and Technology | |
| Defense Advanced Research Projects Agency | |
| U.S. Department of Commerce | |
| Office of Science | |
| Office of Energy Efficiency and Renewable Energy | |
| Vehicle Technologies Program | |
| Argonne National Laboratory | |
| Oak Ridge National Laboratory | |
| Division of Materials Sciences and Engineering | DE-AC05-00OR22725 |