Influence of phonon anharmonicity on Raman spectra of Cu2ZnSn(S,Se)4 polycrystalline thin films through computational study
Abstract Cu2ZnSn(S,Se)4 (CZT(S,Se)) thin films exhibit the characteristics necessary to be effective absorbers in solar cells. In this report, the room temperature experimental Raman scattering spectra, recorded at different excitation wavelengths, are systematically analyzed theoretically using the...
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2025-01-01
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| Online Access: | https://doi.org/10.1038/s41598-024-83117-9 |
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| author | Yurii A. Romaniuk Ivan S. Babichuk Vadym V. Korotyeyev Volodymyr O. Yukhymchuk Volodymyr M. Dzhagan Sergiy V. Virko Mykola O. Semenenko Maksym O. Stetsenko Anton Tiutiunnyk Laura M. Pérez David Laroze |
| author_facet | Yurii A. Romaniuk Ivan S. Babichuk Vadym V. Korotyeyev Volodymyr O. Yukhymchuk Volodymyr M. Dzhagan Sergiy V. Virko Mykola O. Semenenko Maksym O. Stetsenko Anton Tiutiunnyk Laura M. Pérez David Laroze |
| author_sort | Yurii A. Romaniuk |
| collection | DOAJ |
| description | Abstract Cu2ZnSn(S,Se)4 (CZT(S,Se)) thin films exhibit the characteristics necessary to be effective absorbers in solar cells. In this report, the room temperature experimental Raman scattering spectra, recorded at different excitation wavelengths, are systematically analyzed theoretically using the results of DFT harmonic frequencies calculations at the Γ-point for various modifications of kesterite (KS), stannite (ST), and pre-mixed Cu-Au (PMCA) crystal structures. The specific anharmonism‐induced features in the spectra of CZT(S,Se) crystals are identified, and the spectral lineshapes at varied strengths of anharmonic interaction are simulated. A robust agreement between the experimental Raman spectrum and the theoretical results is demonstrated, ensuring the reliability of estimating parameters related to anharmonic effects. Therefore, our findings show that incorporating anharmonism as an additional contribution to the phonon spectra, particularly in non-resonant cases, allows for a more accurate description of the vibrational properties of CZT(S,Se). This could play a crucial role in distinguishing between different phases of CZT(S,Se) materials and open new possibilities for the fabrication of solar cells with enhanced characteristics. |
| format | Article |
| id | doaj-art-58313b5ff9f542fb9a11fbafe3caf848 |
| institution | Kabale University |
| issn | 2045-2322 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Scientific Reports |
| spelling | doaj-art-58313b5ff9f542fb9a11fbafe3caf8482025-01-05T12:13:57ZengNature PortfolioScientific Reports2045-23222025-01-0115111710.1038/s41598-024-83117-9Influence of phonon anharmonicity on Raman spectra of Cu2ZnSn(S,Se)4 polycrystalline thin films through computational studyYurii A. Romaniuk0Ivan S. Babichuk1Vadym V. Korotyeyev2Volodymyr O. Yukhymchuk3Volodymyr M. Dzhagan4Sergiy V. Virko5Mykola O. Semenenko6Maksym O. Stetsenko7Anton Tiutiunnyk8Laura M. Pérez9David Laroze10State Key Laboratory of Precision Spectroscopy, East China Normal UniversityV. Ye Lashkaryov Institute of Semiconductor Physics, NAS of UkraineV. Ye Lashkaryov Institute of Semiconductor Physics, NAS of UkraineV. Ye Lashkaryov Institute of Semiconductor Physics, NAS of UkraineV. Ye Lashkaryov Institute of Semiconductor Physics, NAS of UkraineV. Ye Lashkaryov Institute of Semiconductor Physics, NAS of UkraineV. Ye Lashkaryov Institute of Semiconductor Physics, NAS of UkraineSchool of Science, Westlake UniversityDepartamento de Física, FACI, Universidad de TarapacáDepartamento de Ingeniería Industrial y de Sistemas, Universidad de TarapacáInstituto de Alta Investigación, Universidad de TarapacáAbstract Cu2ZnSn(S,Se)4 (CZT(S,Se)) thin films exhibit the characteristics necessary to be effective absorbers in solar cells. In this report, the room temperature experimental Raman scattering spectra, recorded at different excitation wavelengths, are systematically analyzed theoretically using the results of DFT harmonic frequencies calculations at the Γ-point for various modifications of kesterite (KS), stannite (ST), and pre-mixed Cu-Au (PMCA) crystal structures. The specific anharmonism‐induced features in the spectra of CZT(S,Se) crystals are identified, and the spectral lineshapes at varied strengths of anharmonic interaction are simulated. A robust agreement between the experimental Raman spectrum and the theoretical results is demonstrated, ensuring the reliability of estimating parameters related to anharmonic effects. Therefore, our findings show that incorporating anharmonism as an additional contribution to the phonon spectra, particularly in non-resonant cases, allows for a more accurate description of the vibrational properties of CZT(S,Se). This could play a crucial role in distinguishing between different phases of CZT(S,Se) materials and open new possibilities for the fabrication of solar cells with enhanced characteristics.https://doi.org/10.1038/s41598-024-83117-9CZT(S,Se)KesteriteFermi resonanceRaman spectraAnharmonicityDFT calculation |
| spellingShingle | Yurii A. Romaniuk Ivan S. Babichuk Vadym V. Korotyeyev Volodymyr O. Yukhymchuk Volodymyr M. Dzhagan Sergiy V. Virko Mykola O. Semenenko Maksym O. Stetsenko Anton Tiutiunnyk Laura M. Pérez David Laroze Influence of phonon anharmonicity on Raman spectra of Cu2ZnSn(S,Se)4 polycrystalline thin films through computational study Scientific Reports CZT(S,Se) Kesterite Fermi resonance Raman spectra Anharmonicity DFT calculation |
| title | Influence of phonon anharmonicity on Raman spectra of Cu2ZnSn(S,Se)4 polycrystalline thin films through computational study |
| title_full | Influence of phonon anharmonicity on Raman spectra of Cu2ZnSn(S,Se)4 polycrystalline thin films through computational study |
| title_fullStr | Influence of phonon anharmonicity on Raman spectra of Cu2ZnSn(S,Se)4 polycrystalline thin films through computational study |
| title_full_unstemmed | Influence of phonon anharmonicity on Raman spectra of Cu2ZnSn(S,Se)4 polycrystalline thin films through computational study |
| title_short | Influence of phonon anharmonicity on Raman spectra of Cu2ZnSn(S,Se)4 polycrystalline thin films through computational study |
| title_sort | influence of phonon anharmonicity on raman spectra of cu2znsn s se 4 polycrystalline thin films through computational study |
| topic | CZT(S,Se) Kesterite Fermi resonance Raman spectra Anharmonicity DFT calculation |
| url | https://doi.org/10.1038/s41598-024-83117-9 |
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