Roark Chao, Larry K. Heki, Wesley K. Mills and Jon A. Schuller*,
{"title":"利用Mie共振二聚体增强二维杂化有机-无机钙钛矿的磁偶极子发射","authors":"Roark Chao, Larry K. Heki, Wesley K. Mills and Jon A. Schuller*, ","doi":"10.1021/acsaom.4c0052910.1021/acsaom.4c00529","DOIUrl":null,"url":null,"abstract":"<p >Recently, layered 2D hybrid organic–inorganic perovskites (HOIPs) like butylammonium lead iodide (BA<sub>2</sub>PbI<sub>4</sub>) have been shown to exhibit ultrabright out-of-plane-oriented magnetic dipole (MD<sub>OP</sub>) photoluminescence (PL) arising from self-trapped excitons (STEs). The MD<sub>OP</sub> emission, however, has considerable spectral overlap with the dominant in-plane-oriented electric dipole (ED<sub>IP</sub>) transitions, making it difficult to interrogate STE properties. Here, we theoretically investigate opportunities to use Mie resonator dimers to selectively enhance the MD<sub>OP</sub> emission through the Purcell effect. We calculate relative MD and ED Purcell enhancements at dimer center as well as average values across the dimer geometry. We show that the selective enhancement is excellent at the dimer center enabling nearly pure MD<sub>OP</sub> emission (96%) at the MD emission peak (540 nm) as well as predominant MD<sub>OP</sub> emission (up to 77%) across the entire integrated spectrum (500–600 nm). We subsequently show, however, that away from the dimer center, Purcell enhancement of the relatively weak out-of-plane ED<sub>OP</sub> transitions competes with MD<sub>OP</sub> enhancements, reducing the branching ratio (73% at the MD emission peak, 39% spectrally integrated). Lastly, we calculate how the Mie resonator dimer modifies the PL spectra and emitter radiation pattern. Notably, for volume-averaged dipoles, both MD and ED emissions are mediated via the dimer, producing a single donut-beam-like radiation pattern across the entire emission spectrum. Our results clarify the potential for achieving “pure” MD emission from 2D HOIPs via simple Mie resonator Purcell enhancements and highlight the importance of designing nanophotonic structures that can maintain desired selective enhancements away from high-symmetry points.</p>","PeriodicalId":29803,"journal":{"name":"ACS Applied Optical Materials","volume":"3 3","pages":"737–742 737–742"},"PeriodicalIF":0.0000,"publicationDate":"2025-03-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsaom.4c00529","citationCount":"0","resultStr":"{\"title\":\"Enhancing Magnetic Dipole Emission from 2D Hybrid Organic–Inorganic Perovskites via Mie Resonator Dimers\",\"authors\":\"Roark Chao, Larry K. Heki, Wesley K. Mills and Jon A. Schuller*, \",\"doi\":\"10.1021/acsaom.4c0052910.1021/acsaom.4c00529\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Recently, layered 2D hybrid organic–inorganic perovskites (HOIPs) like butylammonium lead iodide (BA<sub>2</sub>PbI<sub>4</sub>) have been shown to exhibit ultrabright out-of-plane-oriented magnetic dipole (MD<sub>OP</sub>) photoluminescence (PL) arising from self-trapped excitons (STEs). The MD<sub>OP</sub> emission, however, has considerable spectral overlap with the dominant in-plane-oriented electric dipole (ED<sub>IP</sub>) transitions, making it difficult to interrogate STE properties. Here, we theoretically investigate opportunities to use Mie resonator dimers to selectively enhance the MD<sub>OP</sub> emission through the Purcell effect. We calculate relative MD and ED Purcell enhancements at dimer center as well as average values across the dimer geometry. We show that the selective enhancement is excellent at the dimer center enabling nearly pure MD<sub>OP</sub> emission (96%) at the MD emission peak (540 nm) as well as predominant MD<sub>OP</sub> emission (up to 77%) across the entire integrated spectrum (500–600 nm). We subsequently show, however, that away from the dimer center, Purcell enhancement of the relatively weak out-of-plane ED<sub>OP</sub> transitions competes with MD<sub>OP</sub> enhancements, reducing the branching ratio (73% at the MD emission peak, 39% spectrally integrated). Lastly, we calculate how the Mie resonator dimer modifies the PL spectra and emitter radiation pattern. Notably, for volume-averaged dipoles, both MD and ED emissions are mediated via the dimer, producing a single donut-beam-like radiation pattern across the entire emission spectrum. Our results clarify the potential for achieving “pure” MD emission from 2D HOIPs via simple Mie resonator Purcell enhancements and highlight the importance of designing nanophotonic structures that can maintain desired selective enhancements away from high-symmetry points.</p>\",\"PeriodicalId\":29803,\"journal\":{\"name\":\"ACS Applied Optical Materials\",\"volume\":\"3 3\",\"pages\":\"737–742 737–742\"},\"PeriodicalIF\":0.0000,\"publicationDate\":\"2025-03-14\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://pubs.acs.org/doi/epdf/10.1021/acsaom.4c00529\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Applied Optical Materials\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acsaom.4c00529\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"\",\"JCRName\":\"\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Applied Optical Materials","FirstCategoryId":"1085","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acsaom.4c00529","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
Enhancing Magnetic Dipole Emission from 2D Hybrid Organic–Inorganic Perovskites via Mie Resonator Dimers
Recently, layered 2D hybrid organic–inorganic perovskites (HOIPs) like butylammonium lead iodide (BA2PbI4) have been shown to exhibit ultrabright out-of-plane-oriented magnetic dipole (MDOP) photoluminescence (PL) arising from self-trapped excitons (STEs). The MDOP emission, however, has considerable spectral overlap with the dominant in-plane-oriented electric dipole (EDIP) transitions, making it difficult to interrogate STE properties. Here, we theoretically investigate opportunities to use Mie resonator dimers to selectively enhance the MDOP emission through the Purcell effect. We calculate relative MD and ED Purcell enhancements at dimer center as well as average values across the dimer geometry. We show that the selective enhancement is excellent at the dimer center enabling nearly pure MDOP emission (96%) at the MD emission peak (540 nm) as well as predominant MDOP emission (up to 77%) across the entire integrated spectrum (500–600 nm). We subsequently show, however, that away from the dimer center, Purcell enhancement of the relatively weak out-of-plane EDOP transitions competes with MDOP enhancements, reducing the branching ratio (73% at the MD emission peak, 39% spectrally integrated). Lastly, we calculate how the Mie resonator dimer modifies the PL spectra and emitter radiation pattern. Notably, for volume-averaged dipoles, both MD and ED emissions are mediated via the dimer, producing a single donut-beam-like radiation pattern across the entire emission spectrum. Our results clarify the potential for achieving “pure” MD emission from 2D HOIPs via simple Mie resonator Purcell enhancements and highlight the importance of designing nanophotonic structures that can maintain desired selective enhancements away from high-symmetry points.
期刊介绍:
ACS Applied Optical Materials is an international and interdisciplinary forum to publish original experimental and theoretical including simulation and modeling research in optical materials complementing the ACS Applied Materials portfolio. With a focus on innovative applications ACS Applied Optical Materials also complements and expands the scope of existing ACS publications that focus on fundamental aspects of the interaction between light and matter in materials science including ACS Photonics Macromolecules Journal of Physical Chemistry C ACS Nano and Nano Letters.The scope of ACS Applied Optical Materials includes high quality research of an applied nature that integrates knowledge in materials science chemistry physics optical science and engineering.