Delocalized Bi-tetrahedral cluster induced ultralow lattice thermal conductivity in Bi3Ir3O11

Ji, Jialin1; Liu, Zhehong2,3; Dai, Jianhong2,3; Qiu, Di1,4; Yang, Jiong1,4; Xi, Jinyang1,4; Long, Youwen2,3,5; Zhang, Wenqing6,7,8,9

2023-03-01

10.1016/j.mtphys.2023.101005

Materials Today Physics   Impact Factor & Quartile

2542-5293

Low-frequency cluster vibration plays an important role in reducing the lattice thermal conductivity of a system. Here, we show a new type of cluster vibration called "delocalized cluster vibration" that involves a highly symmetric local structure with lone pair electrons and marked impacts on lattice thermal transport. We take a transition-metal oxide Bi3Ir3O11 (two specific Wyckoff positions for Bi: corner-Bi1 and inner-Bi2) as an example, which exhibits counterintuitive low lattice thermal conductivity in metallic materials. Based on first-principles simulations of phonon transport in the Boltzmann transport formulation, this study shows that the four fourth neighbor Bi2 atoms form a regular Bi-tetrahedral cluster (Bi24), which collectively vibrates in certain intercorrelated patterns strongly and induces low-frequency optical phonon modes (-0.77 and-1.06 THz) along with low group velocities. The Bi24-related optical modes interrupt the acoustic vibrations and thus suppress the lattice thermal conductivity to an ultralow value (calculated value is 1.0 W/m center dot K at 300 K). Surprisingly, these Bi2-Bi2 have relatively large distances but significant interatomic force constants, indicating delocalized interactions among Bi24. This work demonstrates that the delocalized cluster vibration plays a significant role in lowering lattice thermal conductivity.

SCI

English

Corresponding

Key Research Project of Zhejiang Laboratory[2021PE0AC02] ; National Key Research and Development Program of China["2021YFB3502200","2021YFA1400300","2018YFA0305700"] ; National Natural Science Foundation of China["52172216","92163212","11934017","11921004"] ; Guangdong Innovation Research Team Project[2017ZT07C062] ; Shenzhen Municipal Key-Lab program[ZDSYS20190902092905285] ; Guangdong Provincial Key-Lab program[2019B030301001] ; Chinese Academy of Sciences[XDB33000000]

Materials Science ; Physics

Materials Science, Multidisciplinary ; Physics, Applied

WOS:000943246100001

ELSEVIER

Web of Science

1.Shanghai Univ, Mat Genome Inst, Shanghai 200444, Peoples R China
2.Chinese Acad Sci, Inst Phys, Beijing Natl Lab Condensed Matter Phys, Beijing 100190, Peoples R China
3.Univ Chinese Acad Sci, Sch Phys Sci, Beijing 100049, Peoples R China
4.Zhejiang Lab, Hangzhou 311100, Zhejiang, Peoples R China
5.Songshan Lake Mat Lab, Dongguan 523808, Guangdong, Peoples R China
6.Southern Univ Sci & Technol, Dept Mat Sci & Engn, Shenzhen 518055, Guangdong, Peoples R China
7.Southern Univ Sci & Technol, Shenzhen Inst Quantum Sci & Technol, Shenzhen 518055, Guangdong, Peoples R China
8.Southern Univ Sci & Technol, Shenzhen Municipal Key Lab Adv Quantum Mat & Devic, Shenzhen 518055, Guangdong, Peoples R China
9.Southern Univ Sci & Technol, Guangdong Prov Key Lab Computat Sci & Mat Design, Shenzhen 518055, Guangdong, Peoples R China

Ji, Jialin,Liu, Zhehong,Dai, Jianhong,et al. Delocalized Bi-tetrahedral cluster induced ultralow lattice thermal conductivity in Bi3Ir3O11[J]. Materials Today Physics,2023,32.

Ji, Jialin.,Liu, Zhehong.,Dai, Jianhong.,Qiu, Di.,Yang, Jiong.,...&Zhang, Wenqing.(2023).Delocalized Bi-tetrahedral cluster induced ultralow lattice thermal conductivity in Bi3Ir3O11.Materials Today Physics,32.

Ji, Jialin,et al."Delocalized Bi-tetrahedral cluster induced ultralow lattice thermal conductivity in Bi3Ir3O11".Materials Today Physics 32(2023).