Structural and electronic features enabling delocalized charge-carriers in CuSbSe 2
Abstract Inorganic semiconductors based on heavy pnictogen cations (Sb3+ and Bi3+) have gained significant attention as potential nontoxic and stable alternatives to lead-halide perovskites for solar cell applications. A limitation of these novel materials, which is being increasingly commonly found...
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| Format: | Article |
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Nature Portfolio
2025-01-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-024-55254-2 |
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| author | Yuchen Fu Hugh Lohan Marcello Righetto Yi-Teng Huang Seán R. Kavanagh Chang-Woo Cho Szymon J. Zelewski Young Won Woo Harry Demetriou Martyn A. McLachlan Sandrine Heutz Benjamin A. Piot David O. Scanlon Akshay Rao Laura M. Herz Aron Walsh Robert L. Z. Hoye |
| author_facet | Yuchen Fu Hugh Lohan Marcello Righetto Yi-Teng Huang Seán R. Kavanagh Chang-Woo Cho Szymon J. Zelewski Young Won Woo Harry Demetriou Martyn A. McLachlan Sandrine Heutz Benjamin A. Piot David O. Scanlon Akshay Rao Laura M. Herz Aron Walsh Robert L. Z. Hoye |
| author_sort | Yuchen Fu |
| collection | DOAJ |
| description | Abstract Inorganic semiconductors based on heavy pnictogen cations (Sb3+ and Bi3+) have gained significant attention as potential nontoxic and stable alternatives to lead-halide perovskites for solar cell applications. A limitation of these novel materials, which is being increasingly commonly found, is carrier localization, which substantially reduces mobilities and diffusion lengths. Herein, CuSbSe2 is investigated and discovered to have delocalized free carriers, as shown through optical pump terahertz probe spectroscopy and temperature-dependent mobility measurements. Using a combination of theory and experiment, the critical enabling factors are found to be: 1) having a layered structure, which allows distortions to the unit cell during the propagation of an acoustic wave to be relaxed in the interlayer gaps, with minimal changes in bond length, thus limiting deformation potentials; 2) favourable quasi-bonding interactions across the interlayer gap giving rise to higher electronic dimensionality; 3) Born effective charges not being anomalously high, which, combined with the small bandgap ( $$\le$$ ≤ 1.2 eV), result in a low ionic contribution to the dielectric constant compared to the electronic contribution, thus reducing the strength of Fröhlich coupling. These insights can drive forward the rational discovery of perovskite-inspired materials that can avoid carrier localization. |
| format | Article |
| id | doaj-art-a8ee9d710c284c53b7abe2f8ff79e189 |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-a8ee9d710c284c53b7abe2f8ff79e1892025-01-05T12:38:59ZengNature PortfolioNature Communications2041-17232025-01-0116111610.1038/s41467-024-55254-2Structural and electronic features enabling delocalized charge-carriers in CuSbSe 2Yuchen Fu0Hugh Lohan1Marcello Righetto2Yi-Teng Huang3Seán R. Kavanagh4Chang-Woo Cho5Szymon J. Zelewski6Young Won Woo7Harry Demetriou8Martyn A. McLachlan9Sandrine Heutz10Benjamin A. Piot11David O. Scanlon12Akshay Rao13Laura M. Herz14Aron Walsh15Robert L. Z. Hoye16Inorganic Chemistry Laboratory, University of Oxford, South Parks RoadInorganic Chemistry Laboratory, University of Oxford, South Parks RoadDepartment of Physics, University of Oxford, Clarendon Laboratory, Parks RoadInorganic Chemistry Laboratory, University of Oxford, South Parks RoadHarvard University Center for the Environment, CambridgeLaboratoire National des Champs Magnétiques Intenses, CNRS, LNCMI, Université Grenoble Alpes, Université Toulouse 3, INSA Toulouse, EMFLCavendish Laboratory, University of Cambridge, JJ Thomson AveDepartment of Materials and Centre for Processable Electronics, Imperial College London, Exhibition RoadDepartment of Materials and Centre for Processable Electronics, Imperial College London, Exhibition RoadDepartment of Materials, Imperial College LondonDepartment of Materials and Centre for Processable Electronics, Imperial College London, Exhibition RoadLaboratoire National des Champs Magnétiques Intenses, CNRS, LNCMI, Université Grenoble Alpes, Université Toulouse 3, INSA Toulouse, EMFLSchool of Chemistry, University of BirminghamCavendish Laboratory, University of Cambridge, JJ Thomson AveDepartment of Physics, University of Oxford, Clarendon Laboratory, Parks RoadDepartment of Materials and Centre for Processable Electronics, Imperial College London, Exhibition RoadInorganic Chemistry Laboratory, University of Oxford, South Parks RoadAbstract Inorganic semiconductors based on heavy pnictogen cations (Sb3+ and Bi3+) have gained significant attention as potential nontoxic and stable alternatives to lead-halide perovskites for solar cell applications. A limitation of these novel materials, which is being increasingly commonly found, is carrier localization, which substantially reduces mobilities and diffusion lengths. Herein, CuSbSe2 is investigated and discovered to have delocalized free carriers, as shown through optical pump terahertz probe spectroscopy and temperature-dependent mobility measurements. Using a combination of theory and experiment, the critical enabling factors are found to be: 1) having a layered structure, which allows distortions to the unit cell during the propagation of an acoustic wave to be relaxed in the interlayer gaps, with minimal changes in bond length, thus limiting deformation potentials; 2) favourable quasi-bonding interactions across the interlayer gap giving rise to higher electronic dimensionality; 3) Born effective charges not being anomalously high, which, combined with the small bandgap ( $$\le$$ ≤ 1.2 eV), result in a low ionic contribution to the dielectric constant compared to the electronic contribution, thus reducing the strength of Fröhlich coupling. These insights can drive forward the rational discovery of perovskite-inspired materials that can avoid carrier localization.https://doi.org/10.1038/s41467-024-55254-2 |
| spellingShingle | Yuchen Fu Hugh Lohan Marcello Righetto Yi-Teng Huang Seán R. Kavanagh Chang-Woo Cho Szymon J. Zelewski Young Won Woo Harry Demetriou Martyn A. McLachlan Sandrine Heutz Benjamin A. Piot David O. Scanlon Akshay Rao Laura M. Herz Aron Walsh Robert L. Z. Hoye Structural and electronic features enabling delocalized charge-carriers in CuSbSe 2 Nature Communications |
| title | Structural and electronic features enabling delocalized charge-carriers in CuSbSe 2 |
| title_full | Structural and electronic features enabling delocalized charge-carriers in CuSbSe 2 |
| title_fullStr | Structural and electronic features enabling delocalized charge-carriers in CuSbSe 2 |
| title_full_unstemmed | Structural and electronic features enabling delocalized charge-carriers in CuSbSe 2 |
| title_short | Structural and electronic features enabling delocalized charge-carriers in CuSbSe 2 |
| title_sort | structural and electronic features enabling delocalized charge carriers in cusbse 2 |
| url | https://doi.org/10.1038/s41467-024-55254-2 |
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