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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Science Press
2025-03-01
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| Series: | National Science Open |
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| Online Access: | https://www.sciengine.com/doi/10.1360/nso/20250004 |
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| author | 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 |
| author_facet | 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 |
| author_sort | Chen Pengpeng |
| collection | DOAJ |
| description | 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>. |
| format | Article |
| id | doaj-art-eef9cf359d7e4e39b12beb1eb9d02a47 |
| institution | OA Journals |
| issn | 2097-1168 |
| language | English |
| publishDate | 2025-03-01 |
| publisher | Science Press |
| record_format | Article |
| series | National Science Open |
| spelling | doaj-art-eef9cf359d7e4e39b12beb1eb9d02a472025-08-20T01:54:57ZengScience PressNational Science Open2097-11682025-03-01410.1360/nso/20250004eb33e642Off-centering effect and crystal symmetry modification lead to high thermoelectric performance in diamondoid Cu<sub>2</sub>SnSe<sub>3</sub>Chen Pengpeng0Bai Shulin1Wen Yi2Li Yichen3Zhao Zihao4Gao Dezheng5Huang Houdong6Hu Yixuan7Gao Tian8Wang Lei9Zhan Shaoping10Gao Xiang11Su Xianli12Xie Hongyao13Zhao Li-Dong14["School of Materials Science and Engineering, Beihang University, Beijing 100191, China"]["School of Materials Science and Engineering, Beihang University, Beijing 100191, China","Center for Bioinspired Science and Technology, Hangzhou International Innovation Institute, Beihang University, Hangzhou 311115, China"]["School of Materials Science and Engineering, Beihang University, Beijing 100191, China"]["School of Materials Science and Engineering, Beihang University, Beijing 100191, China"]["School of Materials Science and Engineering, Beihang University, Beijing 100191, China"]["School of Materials Science and Engineering, Beihang University, Beijing 100191, China"]["State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China"]["School of Materials Science and Engineering, Beihang University, Beijing 100191, China"]["School of Materials Science and Engineering, Beihang University, Beijing 100191, China"]["School of Materials Science and Engineering, Beihang University, Beijing 100191, China"]["School of Materials Science and Engineering, Beihang University, Beijing 100191, China"]["Center for High Pressure Science and Technology Advanced Research (HPSTAR), Beijing 100094, China"]["State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China"]["School of Materials Science and Engineering, Beihang University, Beijing 100191, China"]["School of Materials Science and Engineering, Beihang University, Beijing 100191, China","Center for Bioinspired Science and Technology, Hangzhou International Innovation Institute, Beihang University, Hangzhou 311115, China"]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>.https://www.sciengine.com/doi/10.1360/nso/20250004thermoelectriccrystal structure transitionoff-centering behaviorlocal symmetry breaking |
| spellingShingle | 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 Off-centering effect and crystal symmetry modification lead to high thermoelectric performance in diamondoid Cu<sub>2</sub>SnSe<sub>3</sub> National Science Open thermoelectric crystal structure transition off-centering behavior local symmetry breaking |
| title | Off-centering effect and crystal symmetry modification lead to high thermoelectric performance in diamondoid Cu<sub>2</sub>SnSe<sub>3</sub> |
| title_full | Off-centering effect and crystal symmetry modification lead to high thermoelectric performance in diamondoid Cu<sub>2</sub>SnSe<sub>3</sub> |
| title_fullStr | Off-centering effect and crystal symmetry modification lead to high thermoelectric performance in diamondoid Cu<sub>2</sub>SnSe<sub>3</sub> |
| title_full_unstemmed | Off-centering effect and crystal symmetry modification lead to high thermoelectric performance in diamondoid Cu<sub>2</sub>SnSe<sub>3</sub> |
| title_short | Off-centering effect and crystal symmetry modification lead to high thermoelectric performance in diamondoid Cu<sub>2</sub>SnSe<sub>3</sub> |
| title_sort | off centering effect and crystal symmetry modification lead to high thermoelectric performance in diamondoid cu sub 2 sub snse sub 3 sub |
| topic | thermoelectric crystal structure transition off-centering behavior local symmetry breaking |
| url | https://www.sciengine.com/doi/10.1360/nso/20250004 |
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