Xinlei Zhang, Jing Leng, Qi Sun, Hui Cheng, Fengke Sun, Yejun Xiao, Yan Xu, Wenming Tian, Shengye Jin
{"title":"波函数工程抑制mn掺杂核壳钙钛矿纳米晶体中的俄歇交叉弛豫","authors":"Xinlei Zhang, Jing Leng, Qi Sun, Hui Cheng, Fengke Sun, Yejun Xiao, Yan Xu, Wenming Tian, Shengye Jin","doi":"10.1021/acs.jpclett.5c00005","DOIUrl":null,"url":null,"abstract":"Mn-doped perovskite nanocrystals (NCs) exhibit great application potential because of their unique optical properties. However, the long-lived nature of excited Mn<sup>2+</sup> easily leads to the coexistence of excited Mn<sup>2+</sup> and host excitons in a single NC, which inevitably induces an Auger cross relaxation between them, thus significantly limiting the luminescent efficiency of Mn<sup>2+</sup> due to its competition with internal energy transfer. Herein, we design and prepare a kind of Mn-doped core–shell CsPbCl<sub>3</sub>@Cs<sub>4</sub>PbCl<sub>6</sub> perovskite NC with Mn<sup>2+</sup> doped only in the shell layer, which is expected to suppress this Auger process by spatially separating the electronic wave functions. By using pump–pump–probe transient absorption spectroscopy, we demonstrate that the core–shell structure effectively suppresses the Auger process with the Auger relaxation time notably extended from 12.1 to 148.3 ps. Our finding offers an effective strategy to suppress this Auger process in Mn-doped NCs, which is greatly significant for improving their luminescent efficiency.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"133 1","pages":""},"PeriodicalIF":4.6000,"publicationDate":"2025-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Suppression of Auger Cross Relaxation in Mn-Doped Core–Shell Perovskite Nanocrystals via Wave Function Engineering\",\"authors\":\"Xinlei Zhang, Jing Leng, Qi Sun, Hui Cheng, Fengke Sun, Yejun Xiao, Yan Xu, Wenming Tian, Shengye Jin\",\"doi\":\"10.1021/acs.jpclett.5c00005\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Mn-doped perovskite nanocrystals (NCs) exhibit great application potential because of their unique optical properties. However, the long-lived nature of excited Mn<sup>2+</sup> easily leads to the coexistence of excited Mn<sup>2+</sup> and host excitons in a single NC, which inevitably induces an Auger cross relaxation between them, thus significantly limiting the luminescent efficiency of Mn<sup>2+</sup> due to its competition with internal energy transfer. Herein, we design and prepare a kind of Mn-doped core–shell CsPbCl<sub>3</sub>@Cs<sub>4</sub>PbCl<sub>6</sub> perovskite NC with Mn<sup>2+</sup> doped only in the shell layer, which is expected to suppress this Auger process by spatially separating the electronic wave functions. By using pump–pump–probe transient absorption spectroscopy, we demonstrate that the core–shell structure effectively suppresses the Auger process with the Auger relaxation time notably extended from 12.1 to 148.3 ps. Our finding offers an effective strategy to suppress this Auger process in Mn-doped NCs, which is greatly significant for improving their luminescent efficiency.\",\"PeriodicalId\":62,\"journal\":{\"name\":\"The Journal of Physical Chemistry Letters\",\"volume\":\"133 1\",\"pages\":\"\"},\"PeriodicalIF\":4.6000,\"publicationDate\":\"2025-02-04\",\"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://doi.org/10.1021/acs.jpclett.5c00005\",\"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://doi.org/10.1021/acs.jpclett.5c00005","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Suppression of Auger Cross Relaxation in Mn-Doped Core–Shell Perovskite Nanocrystals via Wave Function Engineering
Mn-doped perovskite nanocrystals (NCs) exhibit great application potential because of their unique optical properties. However, the long-lived nature of excited Mn2+ easily leads to the coexistence of excited Mn2+ and host excitons in a single NC, which inevitably induces an Auger cross relaxation between them, thus significantly limiting the luminescent efficiency of Mn2+ due to its competition with internal energy transfer. Herein, we design and prepare a kind of Mn-doped core–shell CsPbCl3@Cs4PbCl6 perovskite NC with Mn2+ doped only in the shell layer, which is expected to suppress this Auger process by spatially separating the electronic wave functions. By using pump–pump–probe transient absorption spectroscopy, we demonstrate that the core–shell structure effectively suppresses the Auger process with the Auger relaxation time notably extended from 12.1 to 148.3 ps. Our finding offers an effective strategy to suppress this Auger process in Mn-doped NCs, which is greatly significant for improving their luminescent efficiency.
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.