{"title":"通过简便的 pH 值调节操纵手性无机纳米系统中的激子自旋动力学并从机理上理解其原理","authors":"Qinglong Wu, Shenlong Jiang, Qun Zhang, Yi Luo","doi":"10.1002/adom.202400583","DOIUrl":null,"url":null,"abstract":"<p>This study demonstrates effective manipulation of exciton spin dynamics in a prototypical chiral inorganic nanosystem, i.e., cadmium selenide (CdSe) nanosheets capped with chiral cysteine ligands in aqueous solution, via facile pH-regulation that can directly modify the electronic coupling between CdSe and cysteine's thiol group through Cd─S bonding. The comparative scrutiny by using transient circular dichroism spectroscopy enables to decipher the pertinent mechanisms behind the pH-regulated spin-flip dynamics. The hole-trapping interaction between the valence-band heavy-hole spin state of CdSe and the cysteine-induced “extrinsic” surface state is found to play a dominant role in prolonging the hole spin relaxation lifetime (by more than threefold). This study also demonstrates a relevant application in modulating the sensitivity of circularly polarized light detection. This work sets a paradigm for harnessing the elusive interactions in chiral inorganic nanosystems to achieve desired spin-polarization regulation, refreshing the fundamental understanding about the mechanisms of spin dynamics involved therein.</p>","PeriodicalId":116,"journal":{"name":"Advanced Optical Materials","volume":null,"pages":null},"PeriodicalIF":8.0000,"publicationDate":"2024-06-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Manipulation and Mechanistic Understanding of Exciton Spin Dynamics in a Chiral Inorganic Nanosystem via Facile pH-Regulation\",\"authors\":\"Qinglong Wu, Shenlong Jiang, Qun Zhang, Yi Luo\",\"doi\":\"10.1002/adom.202400583\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>This study demonstrates effective manipulation of exciton spin dynamics in a prototypical chiral inorganic nanosystem, i.e., cadmium selenide (CdSe) nanosheets capped with chiral cysteine ligands in aqueous solution, via facile pH-regulation that can directly modify the electronic coupling between CdSe and cysteine's thiol group through Cd─S bonding. The comparative scrutiny by using transient circular dichroism spectroscopy enables to decipher the pertinent mechanisms behind the pH-regulated spin-flip dynamics. The hole-trapping interaction between the valence-band heavy-hole spin state of CdSe and the cysteine-induced “extrinsic” surface state is found to play a dominant role in prolonging the hole spin relaxation lifetime (by more than threefold). This study also demonstrates a relevant application in modulating the sensitivity of circularly polarized light detection. This work sets a paradigm for harnessing the elusive interactions in chiral inorganic nanosystems to achieve desired spin-polarization regulation, refreshing the fundamental understanding about the mechanisms of spin dynamics involved therein.</p>\",\"PeriodicalId\":116,\"journal\":{\"name\":\"Advanced Optical Materials\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":8.0000,\"publicationDate\":\"2024-06-11\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Advanced Optical Materials\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://onlinelibrary.wiley.com/doi/10.1002/adom.202400583\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"MATERIALS SCIENCE, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Advanced Optical Materials","FirstCategoryId":"88","ListUrlMain":"https://onlinelibrary.wiley.com/doi/10.1002/adom.202400583","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}
Manipulation and Mechanistic Understanding of Exciton Spin Dynamics in a Chiral Inorganic Nanosystem via Facile pH-Regulation
This study demonstrates effective manipulation of exciton spin dynamics in a prototypical chiral inorganic nanosystem, i.e., cadmium selenide (CdSe) nanosheets capped with chiral cysteine ligands in aqueous solution, via facile pH-regulation that can directly modify the electronic coupling between CdSe and cysteine's thiol group through Cd─S bonding. The comparative scrutiny by using transient circular dichroism spectroscopy enables to decipher the pertinent mechanisms behind the pH-regulated spin-flip dynamics. The hole-trapping interaction between the valence-band heavy-hole spin state of CdSe and the cysteine-induced “extrinsic” surface state is found to play a dominant role in prolonging the hole spin relaxation lifetime (by more than threefold). This study also demonstrates a relevant application in modulating the sensitivity of circularly polarized light detection. This work sets a paradigm for harnessing the elusive interactions in chiral inorganic nanosystems to achieve desired spin-polarization regulation, refreshing the fundamental understanding about the mechanisms of spin dynamics involved therein.
期刊介绍:
Advanced Optical Materials, part of the esteemed Advanced portfolio, is a unique materials science journal concentrating on all facets of light-matter interactions. For over a decade, it has been the preferred optical materials journal for significant discoveries in photonics, plasmonics, metamaterials, and more. The Advanced portfolio from Wiley is a collection of globally respected, high-impact journals that disseminate the best science from established and emerging researchers, aiding them in fulfilling their mission and amplifying the reach of their scientific discoveries.