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  4. Unravelling ultralow thermal conductivity in perovskite Cs2AgBiBr6: dominant wave-like phonon tunnelling and strong anharmonicity
 
research article

Unravelling ultralow thermal conductivity in perovskite Cs2AgBiBr6: dominant wave-like phonon tunnelling and strong anharmonicity

Zheng, Jiongzhi
•
Lin, Changpeng  
•
Lin, Chongjia
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February 6, 2024
Npj Computational Materials

Understanding the lattice dynamics and heat transport physics in the lead-free halide double perovskites remains an outstanding challenge due to their lattice dynamical instability and strong anharmonicity. In this work, we investigate the microscopic mechanisms of anharmonic lattice dynamics and thermal transport in lead-free halide double perovskite Cs2AgBiBr6 from first principles. We combine self-consistent phonon calculations with bubble diagram correction and a unified theory of lattice thermal transport that considers both the particle-like phonon propagation and wave-like tunnelling of phonons. An ultra-low thermal conductivity at room temperature (similar to 0.21 Wm(-1)K(-1)) is predicted with weak temperature dependence( similar to T-0.34), in sharp contrast to the conventional similar to T-1 dependence. Particularly, the vibrational properties of Cs2AgBiBr6 are featured by strong anharmonicity and wave-like tunnelling of phonons. Anharmonic phonon renormalization from both the cubic and quartic anharmonicities are found essential in precisely predicting the phase transition temperature in Cs2AgBiBr6 while the negative phonon energy shifts induced by cubic anharmonicity has a significant influence on particle-like phonon propagation. Further, the contribution of the wave-like tunnelling to the total thermal conductivity surpasses that of the particle-like propagation above around 310 K, indicating the breakdown of the phonon gas picture conventionally used in the Peierls-Boltzmann Transport Equation. Importantly, further including four-phonon scatterings is required in achieving the dominance of wave-like tunnelling, as compared to the dominant particle-like propagation channel when considering only three-phonon scatterings. Our work highlights the importance of lattice anharmonicity and wave-like tunnelling of phonons in the thermal transport in lead-free halide double perovskites.

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Type
research article
DOI
10.1038/s41524-024-01211-y
Web of Science ID

WOS:001158591600001

Author(s)
Zheng, Jiongzhi
Lin, Changpeng  
Lin, Chongjia
Hautier, Geoffroy
Guo, Ruiqiang
Huang, Baoling
Date Issued

2024-02-06

Publisher

Nature Portfolio

Published in
Npj Computational Materials
Volume

10

Issue

1

Start page

30

Subjects

Physical Sciences

•

Technology

•

Transport

•

Scattering

•

Hole

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
THEOS  
FunderGrant Number

the Science and Technology Planning Project of Guangdong Province, China (Grant No. 2017A050506053), the Science and Technology Program of Guangzhou (No. 201704030107), and the Hong Kong General Research Fund (Grants No. 16214217 and No. 16206020). This pa

2017A050506053

Science and Technology Planning Project of Guangdong Province, China

201704030107

Science and Technology Program of Guangzhou

16214217

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Available on Infoscience
February 23, 2024
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/205532
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