Shovon Chatterjee, Puspal Mukherjee*, Arghya Sen and Pratik Sen*,
{"title":"Cs3Cu2I5 包晶中短寿命高能发射态的证据和自俘获激子的三重子特性","authors":"Shovon Chatterjee, Puspal Mukherjee*, Arghya Sen and Pratik Sen*, ","doi":"10.1021/acs.jpclett.4c00511","DOIUrl":null,"url":null,"abstract":"<p >Cs<sub>3</sub>Cu<sub>2</sub>I<sub>5</sub> perovskite displays a Stokes-shifted photoluminescence (PL) at 445 nm, attributed to the self-trapped excitons (STEs). Unlike that observed in other perovskite materials, the free-exciton emission is not evidenced in this case. Herein, we reveal the existence of a short-lived high-energy emission centered around 375 nm through the reconstruction of time-resolved emission spectra (TRES), which is independent of the shape/size of Cs<sub>3</sub>Cu<sub>2</sub>I<sub>5</sub> perovskite. This high-energy emission is proposed to originate from the free-exciton-derived distorted S1 state of the 0D Cs<sub>3</sub>Cu<sub>2</sub>I<sub>5</sub> moiety. Moreover, STE PL (∼445 nm) was found to have phosphorescence characteristics. Theoretical calculation confirms a facile intersystem crossing at the Franck–Condon geometry, indicating the high lifetime of the STE and its triplet nature. The existence of a high-energy emissive state and the phosphorescent nature of the STE PL band provide valuable insights that could advance our understanding of the photophysics in these materials.</p>","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"15 15","pages":"4191–4196"},"PeriodicalIF":4.6000,"publicationDate":"2024-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Evidence of Short-Lived High-Energy Emissive State and Triplet Character of the Self-Trapped Exciton in Cs3Cu2I5 Perovskite\",\"authors\":\"Shovon Chatterjee, Puspal Mukherjee*, Arghya Sen and Pratik Sen*, \",\"doi\":\"10.1021/acs.jpclett.4c00511\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Cs<sub>3</sub>Cu<sub>2</sub>I<sub>5</sub> perovskite displays a Stokes-shifted photoluminescence (PL) at 445 nm, attributed to the self-trapped excitons (STEs). Unlike that observed in other perovskite materials, the free-exciton emission is not evidenced in this case. Herein, we reveal the existence of a short-lived high-energy emission centered around 375 nm through the reconstruction of time-resolved emission spectra (TRES), which is independent of the shape/size of Cs<sub>3</sub>Cu<sub>2</sub>I<sub>5</sub> perovskite. This high-energy emission is proposed to originate from the free-exciton-derived distorted S1 state of the 0D Cs<sub>3</sub>Cu<sub>2</sub>I<sub>5</sub> moiety. Moreover, STE PL (∼445 nm) was found to have phosphorescence characteristics. Theoretical calculation confirms a facile intersystem crossing at the Franck–Condon geometry, indicating the high lifetime of the STE and its triplet nature. The existence of a high-energy emissive state and the phosphorescent nature of the STE PL band provide valuable insights that could advance our understanding of the photophysics in these materials.</p>\",\"PeriodicalId\":62,\"journal\":{\"name\":\"The Journal of Physical Chemistry Letters\",\"volume\":\"15 15\",\"pages\":\"4191–4196\"},\"PeriodicalIF\":4.6000,\"publicationDate\":\"2024-04-10\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"The Journal of Physical Chemistry Letters\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acs.jpclett.4c00511\",\"RegionNum\":2,\"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 Letters","FirstCategoryId":"1","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acs.jpclett.4c00511","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Evidence of Short-Lived High-Energy Emissive State and Triplet Character of the Self-Trapped Exciton in Cs3Cu2I5 Perovskite
Cs3Cu2I5 perovskite displays a Stokes-shifted photoluminescence (PL) at 445 nm, attributed to the self-trapped excitons (STEs). Unlike that observed in other perovskite materials, the free-exciton emission is not evidenced in this case. Herein, we reveal the existence of a short-lived high-energy emission centered around 375 nm through the reconstruction of time-resolved emission spectra (TRES), which is independent of the shape/size of Cs3Cu2I5 perovskite. This high-energy emission is proposed to originate from the free-exciton-derived distorted S1 state of the 0D Cs3Cu2I5 moiety. Moreover, STE PL (∼445 nm) was found to have phosphorescence characteristics. Theoretical calculation confirms a facile intersystem crossing at the Franck–Condon geometry, indicating the high lifetime of the STE and its triplet nature. The existence of a high-energy emissive state and the phosphorescent nature of the STE PL band provide valuable insights that could advance our understanding of the photophysics in these materials.
期刊介绍：
The Journal of Physical Chemistry (JPC) Letters is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, chemical physicists, physicists, material scientists, and engineers. An important criterion for acceptance is that the paper reports a significant scientific advance and/or physical insight such that rapid publication is essential. Two issues of JPC Letters are published each month.
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