Yuming Li, Yang Liu*, Xuesong Li, Jianxi Yao and Xiaoping Ouyang,
{"title":"空位缺陷对Cs3Cu2I5闪烁体电子和光学性质影响的第一性原理研究","authors":"Yuming Li, Yang Liu*, Xuesong Li, Jianxi Yao and Xiaoping Ouyang, ","doi":"10.1021/acs.jpcc.5c00864","DOIUrl":null,"url":null,"abstract":"<p >Lead-free copper-based halide perovskite Cs<sub>3</sub>Cu<sub>2</sub>I<sub>5</sub> crystals have been recognized as a highly promising material in the field of scintillator materials due to their high quantum yield and fast decay characteristics. Their exceptional optical properties and environmental stability render them highly advantageous for gamma and X-ray detection applications, showcasing significant potential for practical use. To conduct a comprehensive analysis of the impact of irradiation defects on the luminescent performance of Cs<sub>3</sub>Cu<sub>2</sub>I<sub>5</sub> scintillators and their physical mechanisms, this study employs first-principles methods, focusing on the effects of vacancy defects induced by irradiation on the electronic structure and optical properties of Cs<sub>3</sub>Cu<sub>2</sub>I<sub>5</sub> crystals. The research finds that Cs and Cu vacancy defects introduce shallow energy levels within the material’s bandgap, thereby expanding the luminescent pathways of the crystal and significantly enhancing the radiative recombination rate. In contrast, I vacancy defects create deep energy levels in the bandgap, functioning as nonradiative recombination centers, thereby suppressing luminescent performance. Furthermore, the presence of I vacancy defects exacerbates the self-absorption of visible light in Cs<sub>3</sub>Cu<sub>2</sub>I<sub>5</sub> scintillators, resulting in a diminished optical signal reaching the photomultiplier tube, and consequently affecting the overall detection efficiency of the scintillator detector. This study reveals the microscopic mechanisms of damage to Cs<sub>3</sub>Cu<sub>2</sub>I<sub>5</sub> scintillators under high-energy radiation, offering significant theoretical insights for performance optimization and damage protection in practical applications.</p>","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"129 25","pages":"11583–11592"},"PeriodicalIF":3.2000,"publicationDate":"2025-06-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Effect of Vacancy-Defect on the Electronic and Optical Properties of Cs3Cu2I5 Scintillators: A First-Principles Study\",\"authors\":\"Yuming Li, Yang Liu*, Xuesong Li, Jianxi Yao and Xiaoping Ouyang, \",\"doi\":\"10.1021/acs.jpcc.5c00864\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Lead-free copper-based halide perovskite Cs<sub>3</sub>Cu<sub>2</sub>I<sub>5</sub> crystals have been recognized as a highly promising material in the field of scintillator materials due to their high quantum yield and fast decay characteristics. Their exceptional optical properties and environmental stability render them highly advantageous for gamma and X-ray detection applications, showcasing significant potential for practical use. To conduct a comprehensive analysis of the impact of irradiation defects on the luminescent performance of Cs<sub>3</sub>Cu<sub>2</sub>I<sub>5</sub> scintillators and their physical mechanisms, this study employs first-principles methods, focusing on the effects of vacancy defects induced by irradiation on the electronic structure and optical properties of Cs<sub>3</sub>Cu<sub>2</sub>I<sub>5</sub> crystals. The research finds that Cs and Cu vacancy defects introduce shallow energy levels within the material’s bandgap, thereby expanding the luminescent pathways of the crystal and significantly enhancing the radiative recombination rate. In contrast, I vacancy defects create deep energy levels in the bandgap, functioning as nonradiative recombination centers, thereby suppressing luminescent performance. Furthermore, the presence of I vacancy defects exacerbates the self-absorption of visible light in Cs<sub>3</sub>Cu<sub>2</sub>I<sub>5</sub> scintillators, resulting in a diminished optical signal reaching the photomultiplier tube, and consequently affecting the overall detection efficiency of the scintillator detector. This study reveals the microscopic mechanisms of damage to Cs<sub>3</sub>Cu<sub>2</sub>I<sub>5</sub> scintillators under high-energy radiation, offering significant theoretical insights for performance optimization and damage protection in practical applications.</p>\",\"PeriodicalId\":61,\"journal\":{\"name\":\"The Journal of Physical Chemistry C\",\"volume\":\"129 25\",\"pages\":\"11583–11592\"},\"PeriodicalIF\":3.2000,\"publicationDate\":\"2025-06-11\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"The Journal of Physical Chemistry C\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acs.jpcc.5c00864\",\"RegionNum\":3,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"The Journal of Physical Chemistry C","FirstCategoryId":"1","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acs.jpcc.5c00864","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Effect of Vacancy-Defect on the Electronic and Optical Properties of Cs3Cu2I5 Scintillators: A First-Principles Study
Lead-free copper-based halide perovskite Cs3Cu2I5 crystals have been recognized as a highly promising material in the field of scintillator materials due to their high quantum yield and fast decay characteristics. Their exceptional optical properties and environmental stability render them highly advantageous for gamma and X-ray detection applications, showcasing significant potential for practical use. To conduct a comprehensive analysis of the impact of irradiation defects on the luminescent performance of Cs3Cu2I5 scintillators and their physical mechanisms, this study employs first-principles methods, focusing on the effects of vacancy defects induced by irradiation on the electronic structure and optical properties of Cs3Cu2I5 crystals. The research finds that Cs and Cu vacancy defects introduce shallow energy levels within the material’s bandgap, thereby expanding the luminescent pathways of the crystal and significantly enhancing the radiative recombination rate. In contrast, I vacancy defects create deep energy levels in the bandgap, functioning as nonradiative recombination centers, thereby suppressing luminescent performance. Furthermore, the presence of I vacancy defects exacerbates the self-absorption of visible light in Cs3Cu2I5 scintillators, resulting in a diminished optical signal reaching the photomultiplier tube, and consequently affecting the overall detection efficiency of the scintillator detector. This study reveals the microscopic mechanisms of damage to Cs3Cu2I5 scintillators under high-energy radiation, offering significant theoretical insights for performance optimization and damage protection in practical applications.
期刊介绍:
The Journal of Physical Chemistry A/B/C is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, and chemical physicists.