Off-centering effect and crystal symmetry modification lead to high thermoelectric performance in diamondoid Cu<sub>2</sub>SnSe<sub>3</sub>

Recently, dimensionless figure of merit (ZT) beyond 1.0 has been demonstrated in diamondoid Cu<sub>2</sub>SnSe<sub>3</sub>, positioning it as a low-cost and ecofriendly thermoelectric alternative, and sparking intense interest in further optimizing its thermoelectric properti...

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Main Authors: Chen Pengpeng, Bai Shulin, Wen Yi, Li Yichen, Zhao Zihao, Gao Dezheng, Huang Houdong, Hu Yixuan, Gao Tian, Wang Lei, Zhan Shaoping, Gao Xiang, Su Xianli, Xie Hongyao, Zhao Li-Dong
Format: Article
Language:English
Published: Science Press 2025-03-01
Series:National Science Open
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Online Access:https://www.sciengine.com/doi/10.1360/nso/20250004
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Summary:Recently, dimensionless figure of merit (ZT) beyond 1.0 has been demonstrated in diamondoid Cu<sub>2</sub>SnSe<sub>3</sub>, positioning it as a low-cost and ecofriendly thermoelectric alternative, and sparking intense interest in further optimizing its thermoelectric properties. However, its intrinsic monoclinic structure and the compact packing of tetrahedral coordination lead to a light valence band and high thermal conductivity, which impede further performance improvement in Cu<sub>2</sub>SnSe<sub>3</sub>. Thus, developing effective approaches to altering the local structure of Cu<sub>2</sub>SnSe<sub>3</sub> is important for further optimizing its thermoelectric performance. Herein, we identified and thoroughly investigated the atomic off-centering behavior in Cu<sub>2</sub>SnSe<sub>3</sub>, and demonstrated the electronic and phonon transport properties of Cu<sub>2</sub>SnSe<sub>3</sub> can be significantly enhanced by carefully modifying its monoclinic lattice into a distorted zinc-blende cubic structure via introducing Cd and off-centering Ag elements. This structure transition leads to band convergence and a reduction in the deformation potential of the material, resulting in a 7-fold enhancement in the density-of-state effective mass and an 85% increase in carrier mobility. Additionally, the off-centering effect results in strong acoustic-optical phonon scattering and an ultra-low lattice thermal conductivity of <sc>0.3 W m<sup>−1</sup> K<sup>−1</sup>.</sc> Consequently, a maximum ZT of 1.3 was obtained at <sc>800 K</sc> for the Cu<sub>1.85</sub>Ag<sub>0.15</sub>Sn<sub>0.9</sub>Cd<sub>0.1</sub>Se<sub>3</sub>.
ISSN:2097-1168