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Title: Part-crystalline part-liquid state and rattling-like thermal damping in materials with chemical-bond hierarchy

Understanding thermal and phonon transport in solids has been of great importance in many disciplines such as thermoelectric materials, which usually requires an extremely low lattice thermal conductivity (LTC). Here, by analyzing the finite-temperature structural and vibrational characteristics of typical thermoelectric compounds such as filled skutterudites and Cu 3SbSe 3, we demonstrate a concept of part-crystalline part-liquid state in the compounds with chemical-bond hierarchy, in which certain constituent species weakly bond to other part of the crystal. Such a material could intrinsically manifest the coexistence of rigid crystalline sublattices and other fluctuating noncrystalline sublattices with thermally induced large-amplitude vibrations and even flow of the group of species atoms, leading to atomic-level heterogeneity, mixed part-crystalline part-liquid structure, and thus rattling-like thermal damping due to the collective soft-mode vibrations similar to the Boson peak in amorphous materials. Lastly, the observed abnormal LTC close to the amorphous limit in these materials can only be described by an effective approach that approximately treats the rattling-like damping as a “resonant” phonon scattering.
Authors:
ORCiD logo [1] ;  [2] ;  [3] ;  [4] ;  [3] ;  [5]
  1. Chinese Academy of Sciences (CAS), Shanghai (China). Shanghai Inst. of Ceramics. State Key Lab. of High Performance Ceramics and Superfine Microstructure; East China Normal Univ. (ECNU), Shanghai (China). Dept. of Physics. Inst. of Theoretical Physics
  2. Chinese Academy of Sciences (CAS), Shanghai (China). Shanghai Inst. of Ceramics. State Key Lab. of High Performance Ceramics and Superfine Microstructure
  3. Univ. of Washington, Seattle, WA (United States). Materials Science and Engineering Dept.
  4. East China Normal Univ. (ECNU), Shanghai (China). Dept. of Physics. Inst. of Theoretical Physics
  5. Chinese Academy of Sciences (CAS), Shanghai (China). Shanghai Inst. of Ceramics. State Key Lab. of High Performance Ceramics and Superfine Microstructure; Shanghai Univ. (China). Materials Genome Inst.
Publication Date:
Grant/Contract Number:
FC26-04NT42278; 1235535; 2013CB632501; 11234012; 51121064; 11074074; 11204333; 239201278220051; 20110076110002
Type:
Accepted Manuscript
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Volume: 111; Journal Issue: 42; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences, Washington, DC (United States)
Research Org:
Univ. of Washington, Seattle, WA (United States); East China Normal Univ. (ECNU), Shanghai (China); Chinese Academy of Sciences (CAS), Shanghai (China)
Sponsoring Org:
USDOE; National Science Foundation (NSF); General Motors (United States); National Basic Research Program of China; National Natural Science Foundation of China (NNSFC); East China Normal Univ. (China)
Contributing Orgs:
Shanghai Univ. (China)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; sublattice melting; partial Grüneisen parameter; first principles; anharmonicity
OSTI Identifier:
1348359

Qiu, Wujie, Xi, Lili, Wei, Ping, Ke, Xuezhi, Yang, Jihui, and Zhang, Wenqing. Part-crystalline part-liquid state and rattling-like thermal damping in materials with chemical-bond hierarchy. United States: N. p., Web. doi:10.1073/pnas.1410349111.
Qiu, Wujie, Xi, Lili, Wei, Ping, Ke, Xuezhi, Yang, Jihui, & Zhang, Wenqing. Part-crystalline part-liquid state and rattling-like thermal damping in materials with chemical-bond hierarchy. United States. doi:10.1073/pnas.1410349111.
Qiu, Wujie, Xi, Lili, Wei, Ping, Ke, Xuezhi, Yang, Jihui, and Zhang, Wenqing. 2014. "Part-crystalline part-liquid state and rattling-like thermal damping in materials with chemical-bond hierarchy". United States. doi:10.1073/pnas.1410349111. https://www.osti.gov/servlets/purl/1348359.
@article{osti_1348359,
title = {Part-crystalline part-liquid state and rattling-like thermal damping in materials with chemical-bond hierarchy},
author = {Qiu, Wujie and Xi, Lili and Wei, Ping and Ke, Xuezhi and Yang, Jihui and Zhang, Wenqing},
abstractNote = {Understanding thermal and phonon transport in solids has been of great importance in many disciplines such as thermoelectric materials, which usually requires an extremely low lattice thermal conductivity (LTC). Here, by analyzing the finite-temperature structural and vibrational characteristics of typical thermoelectric compounds such as filled skutterudites and Cu3SbSe3, we demonstrate a concept of part-crystalline part-liquid state in the compounds with chemical-bond hierarchy, in which certain constituent species weakly bond to other part of the crystal. Such a material could intrinsically manifest the coexistence of rigid crystalline sublattices and other fluctuating noncrystalline sublattices with thermally induced large-amplitude vibrations and even flow of the group of species atoms, leading to atomic-level heterogeneity, mixed part-crystalline part-liquid structure, and thus rattling-like thermal damping due to the collective soft-mode vibrations similar to the Boson peak in amorphous materials. Lastly, the observed abnormal LTC close to the amorphous limit in these materials can only be described by an effective approach that approximately treats the rattling-like damping as a “resonant” phonon scattering.},
doi = {10.1073/pnas.1410349111},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 42,
volume = 111,
place = {United States},
year = {2014},
month = {10}
}