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Title: Collective-Goldstone-mode-induced ultralow lattice thermal conductivity in Sn-filled skutterudite SnFe 4 Sb 12

Abstract

Here, we demonstrate that the concept of Goldstone bosons can be exploited for phonon control and thermal conductivity reduction of materials. By studying lattice dynamics of the Sn filled skutterudite SnFe 4Sb 12, we find Sn off-centers in its coordination cage in contrast to the common rare earth fillers. This leads to low-frequency Goldstone-like modes below 1 THz associated mainly with Sn motions. Importantly, these involve collective motion of other atoms, especially Sb, in the host skutterudite lattice. The optical modes transversing to the Sn off-centering direction are identified as Goldstone type modes in association with a three-dimensional Mexican-hat-like potential energy surface. The interaction of these collective Goldstone modes with the host heat-carrying phonons is shown to lead to ultralow lattice thermal conductivity.

Authors:
 [1];  [2];  [2];  [3]
  1. Jilin Univ., Changchun (China). State Key Lab. of Superhard Materials, Key Lab. of Automobile Materials of MOE, and College of Materials Science and Engineering; Univ. of Missouri, Columbia, MO (United States). Dept. of Physics and Astronomy
  2. Jilin Univ., Changchun (China). State Key Lab. of Superhard Materials, Key Lab. of Automobile Materials of MOE, and College of Materials Science and Engineering
  3. Univ. of Missouri, Columbia, MO (United States). Dept. of Physics and Astronomy
Publication Date:
Research Org.:
Univ. of Missouri, Columbia, MO (United States); Energy Frontier Research Centers (EFRC) (United States). Solid-State Solar-Thermal Energy Conversion Center (S3TEC)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1415615
Alternate Identifier(s):
OSTI ID: 1415534
Grant/Contract Number:  
SC0001299; FG02-09ER46577
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 97; Journal Issue: 2; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; Phonons; Bonding; Lattice thermal conductivity

Citation Formats

Fu, Yuhao, He, Xin, Zhang, Lijun, and Singh, David J. Collective-Goldstone-mode-induced ultralow lattice thermal conductivity in Sn-filled skutterudite SnFe4Sb12. United States: N. p., 2018. Web. doi:10.1103/PhysRevB.97.024301.
Fu, Yuhao, He, Xin, Zhang, Lijun, & Singh, David J. Collective-Goldstone-mode-induced ultralow lattice thermal conductivity in Sn-filled skutterudite SnFe4Sb12. United States. doi:10.1103/PhysRevB.97.024301.
Fu, Yuhao, He, Xin, Zhang, Lijun, and Singh, David J. Wed . "Collective-Goldstone-mode-induced ultralow lattice thermal conductivity in Sn-filled skutterudite SnFe4Sb12". United States. doi:10.1103/PhysRevB.97.024301. https://www.osti.gov/servlets/purl/1415615.
@article{osti_1415615,
title = {Collective-Goldstone-mode-induced ultralow lattice thermal conductivity in Sn-filled skutterudite SnFe4Sb12},
author = {Fu, Yuhao and He, Xin and Zhang, Lijun and Singh, David J.},
abstractNote = {Here, we demonstrate that the concept of Goldstone bosons can be exploited for phonon control and thermal conductivity reduction of materials. By studying lattice dynamics of the Sn filled skutterudite SnFe4Sb12, we find Sn off-centers in its coordination cage in contrast to the common rare earth fillers. This leads to low-frequency Goldstone-like modes below 1 THz associated mainly with Sn motions. Importantly, these involve collective motion of other atoms, especially Sb, in the host skutterudite lattice. The optical modes transversing to the Sn off-centering direction are identified as Goldstone type modes in association with a three-dimensional Mexican-hat-like potential energy surface. The interaction of these collective Goldstone modes with the host heat-carrying phonons is shown to lead to ultralow lattice thermal conductivity.},
doi = {10.1103/PhysRevB.97.024301},
journal = {Physical Review B},
issn = {2469-9950},
number = 2,
volume = 97,
place = {United States},
year = {2018},
month = {1}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 2 works
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Figures / Tables:

Figure-1 Figure-1: (a) Structure of SnFe4Sb12 (space group Cm) obtained by total energy minimization. Sn off-centers and bonds with three Sb atoms. Sn is located in the (001) plane (blue) comprised of four Sb. (b, c) Charge density in the (001) plane showing the Sb4 ring and the fillers in SnFe4Sb12more » and LaFe4Sb12. The color range is from 0 (blue) to 0.05 (red) electron/Å3.« less

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    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.