Amorphous-Like Ultralow Thermal Transport in Crystalline Argyrodite Cu₇PS₆

Shen, Xingchen1,2; Ouyang, Niuchang3; Huang, Yuling4; Tung, Yung-Hsiang5,6; Yang, Chun-Chuen6; Faizan, Muhammad7; Perez, Nicolas8; He, Ran8; Sotnikov, Andrei9; Willa, Kristin1; Wang, Chen3; Chen, Yue3; Guilmeau, Emmanuel2

2024-06-01

10.1002/advs.202400258

ADVANCED SCIENCE   影响因子和分区

2198-3844

Due to their amorphous-like ultralow lattice thermal conductivity both below and above the superionic phase transition, crystalline Cu- and Ag-based superionic argyrodites have garnered widespread attention as promising thermoelectric materials. However, despite their intriguing properties, quantifying their lattice thermal conductivities and a comprehensive understanding of the microscopic dynamics that drive these extraordinary properties are still lacking. Here, an integrated experimental and theoretical approach is adopted to reveal the presence of Cu-dominated low-energy optical phonons in the Cu-based argyrodite Cu7PS6. These phonons yield strong acoustic-optical phonon scattering through avoided crossing, enabling ultralow lattice thermal conductivity. The Unified Theory of thermal transport is employed to analyze heat conduction and successfully reproduce the experimental amorphous-like ultralow lattice thermal conductivities, ranging from 0.43 to 0.58 W m(-1) K-1, in the temperature range of 100-400 K. The study reveals that the amorphous-like ultralow thermal conductivity of Cu7PS6 stems from a significantly dominant wave-like conduction mechanism. Moreover, the simulations elucidate the wave-like thermal transport mainly results from the contribution of Cu-associated low-energy overlapping optical phonons. This study highlights the crucial role of low-energy and overlapping optical modes in facilitating amorphous-like ultralow thermal transport, providing a thorough understanding of the underlying complex dynamics of argyrodites.

argyrodite Cu7PS6 crystal structure Cu Diffusion lattice dynamics amorphous-like ultralow thermal transport

SCI ; EI

英语

其他

The WINNINGNormandy Program supported by the Normandy Region[101034329] ; Normandy Region["Y-H","C-C"] ; Helmholtz-OCPC Postdoc program["C-C","2021-2-093-1","2022-1-139-1"] ; National Synchrotron Radiation Research Center Taiwan photon source (NSRRC), Taiwan["112-2112-M-008-028","112-2112-M-008-027"] ; National Science and Technology Council of Taiwan[12350410372]

Chemistry ; Science & Technology - Other Topics ; Materials Science

Chemistry, Multidisciplinary ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary

WOS:001190008500001

WILEY

Web of Science

1.Karlsruhe Inst Technol, Inst Quantum Mat & Technol, D-76021 Karlsruhe, Germany
2.Normandie Univ, CRISMAT, CNRS, ENSICAEN,UNICAEN, F-14000 Caen, France
3.Univ Hong Kong, Dept Mech Engn, Pokfulam Rd, Hong Kong, Peoples R China
4.Southern Univ Sci & Technol SUSTech, Dept Mech & Energy, Shenzhen 518055, Peoples R China
5.Forschungszentrum Julich, Julich Ctr Neutron Sci JCNS, Maier Leibnitz Zentrum MLZ, Lichtenbergstr 1, D-85747 Garching, Germany
6.Natl Cent Univ, Dept Phys, Taoyuan 320317, Taiwan
7.Jilin Univ, Coll Mat Sci & Engn, Changchun 130012, Peoples R China
8.IFW Dresden, Inst Met Mat, D-01069 Dresden, Germany
9.Leibniz IFW Dresden, Inst Solid State Res, D-01069 Dresden, Germany

Shen, Xingchen,Ouyang, Niuchang,Huang, Yuling,et al. Amorphous-Like Ultralow Thermal Transport in Crystalline Argyrodite Cu₇PS₆[J]. ADVANCED SCIENCE,2024,11(22).

Shen, Xingchen.,Ouyang, Niuchang.,Huang, Yuling.,Tung, Yung-Hsiang.,Yang, Chun-Chuen.,...&Guilmeau, Emmanuel.(2024).Amorphous-Like Ultralow Thermal Transport in Crystalline Argyrodite Cu₇PS₆.ADVANCED SCIENCE,11(22).

Shen, Xingchen,et al."Amorphous-Like Ultralow Thermal Transport in Crystalline Argyrodite Cu₇PS₆".ADVANCED SCIENCE 11.22(2024).