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Title: Correlated local dipoles in PbTe

Abstract

We present a combined single-crystal x-ray diffuse scattering and ab-initio molecular dynamics study of lead telluride, PbTe. Well-known for its thermoelectric and narrow-gap semiconducting properties, PbTe recently achieved further notoriety following the report of an unusual off-centering of the lead atoms, accompanied by a local symmetry breaking, on heating. This observation, which was named emphanisis, ignited considerable controversy regarding the details of the underlying local structure and the appropriate interpretation of the total scattering experiments. In this study, we identify an unusual correlated local dipole formation extending over several unit cells with an associated local reduction of the cubic symmetry in both our x-ray diffuse scattering measurements and our molecular dynamics simulations. Importantly, when averaged spatially or temporally, the most probable positions for the ions are at the centers of their coordination polyhedra. Our results therefore clarify the nature of the local symmetry breaking, and reveal the source of the earlier controversy regarding the existence or absence of off-centering. Finally, we provide an interpretation of the behavior in terms of coupled soft optical and acoustic modes, which is linked also to the high thermoelectric performance of PbTe.

Authors:
 [1]; ORCiD logo [2];  [3];  [1];  [1];  [3];  [4];  [1];  [1]
  1. Federal Inst. of Technology, Zurich (Switzerland). Dept. of Materials
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Condensed Matter Physics and Materials Science Dept.
  3. Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry
  4. Columbia Univ., New York, NY (United States). Dept. of Applied Physics and Applied Mathematics; Brookhaven National Lab. (BNL), Upton, NY (United States). Condensed Matter Physics and Materials Science Dept.
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1459170
Alternate Identifier(s):
OSTI ID: 1463047
Report Number(s):
BNL-206808-2018-JAAM
Journal ID: ISSN 2475-9953; TRN: US1901546
Grant/Contract Number:  
SC0012704
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Physical Review Materials
Additional Journal Information:
Journal Volume: 2; Journal Issue: 8; Journal ID: ISSN 2475-9953
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Sangiorgio, Boris, Bozin, Emil S., Malliakas, Christos D., Fechner, Michael, Simonov, Arkadiy, Kanatzidis, Mercouri G., Billinge, Simon J. L., Spaldin, Nicola A., and Weber, Thomas. Correlated local dipoles in PbTe. United States: N. p., 2018. Web. doi:10.1103/PhysRevMaterials.2.085402.
Sangiorgio, Boris, Bozin, Emil S., Malliakas, Christos D., Fechner, Michael, Simonov, Arkadiy, Kanatzidis, Mercouri G., Billinge, Simon J. L., Spaldin, Nicola A., & Weber, Thomas. Correlated local dipoles in PbTe. United States. doi:10.1103/PhysRevMaterials.2.085402.
Sangiorgio, Boris, Bozin, Emil S., Malliakas, Christos D., Fechner, Michael, Simonov, Arkadiy, Kanatzidis, Mercouri G., Billinge, Simon J. L., Spaldin, Nicola A., and Weber, Thomas. Mon . "Correlated local dipoles in PbTe". United States. doi:10.1103/PhysRevMaterials.2.085402.
@article{osti_1459170,
title = {Correlated local dipoles in PbTe},
author = {Sangiorgio, Boris and Bozin, Emil S. and Malliakas, Christos D. and Fechner, Michael and Simonov, Arkadiy and Kanatzidis, Mercouri G. and Billinge, Simon J. L. and Spaldin, Nicola A. and Weber, Thomas},
abstractNote = {We present a combined single-crystal x-ray diffuse scattering and ab-initio molecular dynamics study of lead telluride, PbTe. Well-known for its thermoelectric and narrow-gap semiconducting properties, PbTe recently achieved further notoriety following the report of an unusual off-centering of the lead atoms, accompanied by a local symmetry breaking, on heating. This observation, which was named emphanisis, ignited considerable controversy regarding the details of the underlying local structure and the appropriate interpretation of the total scattering experiments. In this study, we identify an unusual correlated local dipole formation extending over several unit cells with an associated local reduction of the cubic symmetry in both our x-ray diffuse scattering measurements and our molecular dynamics simulations. Importantly, when averaged spatially or temporally, the most probable positions for the ions are at the centers of their coordination polyhedra. Our results therefore clarify the nature of the local symmetry breaking, and reveal the source of the earlier controversy regarding the existence or absence of off-centering. Finally, we provide an interpretation of the behavior in terms of coupled soft optical and acoustic modes, which is linked also to the high thermoelectric performance of PbTe.},
doi = {10.1103/PhysRevMaterials.2.085402},
journal = {Physical Review Materials},
issn = {2475-9953},
number = 8,
volume = 2,
place = {United States},
year = {2018},
month = {7}
}

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