Youngsin Park, Elham Oleiki, Guanhua Ying, Atanu Jana, Mutibah Alanazi, Vitaly Osokin, Sangeun Cho, Robert A. Taylor, Geunsik Lee
{"title":"石墨烯包覆的 CsPbBr3 量子点中由表面等离子体介导的光致发光促进作用","authors":"Youngsin Park, Elham Oleiki, Guanhua Ying, Atanu Jana, Mutibah Alanazi, Vitaly Osokin, Sangeun Cho, Robert A. Taylor, Geunsik Lee","doi":"10.1016/j.apsusc.2024.161601","DOIUrl":null,"url":null,"abstract":"The optical properties of graphene (Gr)-covered CsPbBr<sub>3</sub> quantum dots (QDs) were investigated using micro-photoluminescence spectroscopy, revealing a remarkable three orders of magnitude enhancement in photoluminescence (PL) intensity compared to bare CsPbBr<sub>3</sub> QDs. To elucidate the underlying mechanisms, we combined experimental techniques with density functional theory (DFT) calculations. DFT simulations showed that the graphene layer generates interfacial electrostatic potential barriers when in contact with the CsPbBr<sub>3</sub> surface, impeding carrier leakage from perovskite to graphene and enhancing radiative recombination. Additionally, graphene passivates CsPbBr<sub>3</sub> surface defect states, suppressing nonradiative recombination of photo-generated carriers. Our study also revealed that graphene becomes n-doped upon contact with CsPbBr<sub>3</sub> QDs, activating its plasmon mode. This mode resonantly couples with photo-generated excitons in the perovskite. The momentum mismatch between graphene plasmons and free-space photons is resolved through plasmon scattering at Gr/CsPbBr<sub>3</sub> interface corrugations, facilitating the observed super-bright emission. These findings highlight the critical role of graphene as a top contact in dramatically enhancing CsPbBr<sub>3</sub> QDs’ PL. Our work advances the understanding of graphene-perovskite interfaces and opens new avenues for designing high-efficiency optoelectronic devices. The multifaceted enhancement mechanisms uncovered provide valuable insights for future research in nanophotonics and materials science, potentially leading to breakthroughs in light-emitting technologies.","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":null,"pages":null},"PeriodicalIF":6.3000,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Surface plasmon-mediated photoluminescence boost in graphene-covered CsPbBr3 quantum dots\",\"authors\":\"Youngsin Park, Elham Oleiki, Guanhua Ying, Atanu Jana, Mutibah Alanazi, Vitaly Osokin, Sangeun Cho, Robert A. Taylor, Geunsik Lee\",\"doi\":\"10.1016/j.apsusc.2024.161601\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"The optical properties of graphene (Gr)-covered CsPbBr<sub>3</sub> quantum dots (QDs) were investigated using micro-photoluminescence spectroscopy, revealing a remarkable three orders of magnitude enhancement in photoluminescence (PL) intensity compared to bare CsPbBr<sub>3</sub> QDs. To elucidate the underlying mechanisms, we combined experimental techniques with density functional theory (DFT) calculations. DFT simulations showed that the graphene layer generates interfacial electrostatic potential barriers when in contact with the CsPbBr<sub>3</sub> surface, impeding carrier leakage from perovskite to graphene and enhancing radiative recombination. Additionally, graphene passivates CsPbBr<sub>3</sub> surface defect states, suppressing nonradiative recombination of photo-generated carriers. Our study also revealed that graphene becomes n-doped upon contact with CsPbBr<sub>3</sub> QDs, activating its plasmon mode. This mode resonantly couples with photo-generated excitons in the perovskite. The momentum mismatch between graphene plasmons and free-space photons is resolved through plasmon scattering at Gr/CsPbBr<sub>3</sub> interface corrugations, facilitating the observed super-bright emission. These findings highlight the critical role of graphene as a top contact in dramatically enhancing CsPbBr<sub>3</sub> QDs’ PL. Our work advances the understanding of graphene-perovskite interfaces and opens new avenues for designing high-efficiency optoelectronic devices. The multifaceted enhancement mechanisms uncovered provide valuable insights for future research in nanophotonics and materials science, potentially leading to breakthroughs in light-emitting technologies.\",\"PeriodicalId\":247,\"journal\":{\"name\":\"Applied Surface Science\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":6.3000,\"publicationDate\":\"2024-10-22\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Applied Surface Science\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1016/j.apsusc.2024.161601\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Applied Surface Science","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1016/j.apsusc.2024.161601","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Surface plasmon-mediated photoluminescence boost in graphene-covered CsPbBr3 quantum dots
The optical properties of graphene (Gr)-covered CsPbBr3 quantum dots (QDs) were investigated using micro-photoluminescence spectroscopy, revealing a remarkable three orders of magnitude enhancement in photoluminescence (PL) intensity compared to bare CsPbBr3 QDs. To elucidate the underlying mechanisms, we combined experimental techniques with density functional theory (DFT) calculations. DFT simulations showed that the graphene layer generates interfacial electrostatic potential barriers when in contact with the CsPbBr3 surface, impeding carrier leakage from perovskite to graphene and enhancing radiative recombination. Additionally, graphene passivates CsPbBr3 surface defect states, suppressing nonradiative recombination of photo-generated carriers. Our study also revealed that graphene becomes n-doped upon contact with CsPbBr3 QDs, activating its plasmon mode. This mode resonantly couples with photo-generated excitons in the perovskite. The momentum mismatch between graphene plasmons and free-space photons is resolved through plasmon scattering at Gr/CsPbBr3 interface corrugations, facilitating the observed super-bright emission. These findings highlight the critical role of graphene as a top contact in dramatically enhancing CsPbBr3 QDs’ PL. Our work advances the understanding of graphene-perovskite interfaces and opens new avenues for designing high-efficiency optoelectronic devices. The multifaceted enhancement mechanisms uncovered provide valuable insights for future research in nanophotonics and materials science, potentially leading to breakthroughs in light-emitting technologies.
期刊介绍:
Applied Surface Science covers topics contributing to a better understanding of surfaces, interfaces, nanostructures and their applications. The journal is concerned with scientific research on the atomic and molecular level of material properties determined with specific surface analytical techniques and/or computational methods, as well as the processing of such structures.