{"title":"强耦合有机微腔中的多重相互作用光子模式。","authors":"Felipe Herrera, William L Barnes","doi":"10.1098/rsta.2023.0343","DOIUrl":null,"url":null,"abstract":"<p><p>Room-temperature cavity quantum electrodynamics with molecular materials in optical cavities offers exciting prospects for controlling electronic, nuclear and photonic degrees of freedom for applications in physics, chemistry and materials science. However, achieving strong coupling with molecular ensembles typically requires high molecular densities and substantial electromagnetic-field confinement. These conditions usually involve a significant degree of molecular disorder and a highly structured photonic density of states. It remains unclear to what extent these additional complexities modify the usual physical picture of strong coupling developed for atoms and inorganic semiconductors. Using a microscopic quantum description of molecular ensembles in realistic multimode optical resonators, we show that the emergence of vacuum Rabi splitting in linear spectroscopy is a necessary but not sufficient metric of coherent admixing between light and matter. In low-finesse multi-mode situations, we find that molecular dipoles can be partially hybridized with photonic dissipation channels associated with off-resonant cavity modes. These vacuum-induced dissipative processes ultimately limit the extent of light-matter coherence that the system can sustain.This article is part of the theme issue 'The quantum theory of light'.</p>","PeriodicalId":19879,"journal":{"name":"Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences","volume":"382 2287","pages":"20230343"},"PeriodicalIF":4.3000,"publicationDate":"2024-12-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11667587/pdf/","citationCount":"0","resultStr":"{\"title\":\"Multiple interacting photonic modes in strongly coupled organic microcavities.\",\"authors\":\"Felipe Herrera, William L Barnes\",\"doi\":\"10.1098/rsta.2023.0343\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>Room-temperature cavity quantum electrodynamics with molecular materials in optical cavities offers exciting prospects for controlling electronic, nuclear and photonic degrees of freedom for applications in physics, chemistry and materials science. However, achieving strong coupling with molecular ensembles typically requires high molecular densities and substantial electromagnetic-field confinement. These conditions usually involve a significant degree of molecular disorder and a highly structured photonic density of states. It remains unclear to what extent these additional complexities modify the usual physical picture of strong coupling developed for atoms and inorganic semiconductors. Using a microscopic quantum description of molecular ensembles in realistic multimode optical resonators, we show that the emergence of vacuum Rabi splitting in linear spectroscopy is a necessary but not sufficient metric of coherent admixing between light and matter. In low-finesse multi-mode situations, we find that molecular dipoles can be partially hybridized with photonic dissipation channels associated with off-resonant cavity modes. These vacuum-induced dissipative processes ultimately limit the extent of light-matter coherence that the system can sustain.This article is part of the theme issue 'The quantum theory of light'.</p>\",\"PeriodicalId\":19879,\"journal\":{\"name\":\"Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences\",\"volume\":\"382 2287\",\"pages\":\"20230343\"},\"PeriodicalIF\":4.3000,\"publicationDate\":\"2024-12-30\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11667587/pdf/\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences\",\"FirstCategoryId\":\"103\",\"ListUrlMain\":\"https://doi.org/10.1098/rsta.2023.0343\",\"RegionNum\":3,\"RegionCategory\":\"综合性期刊\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"2024/12/24 0:00:00\",\"PubModel\":\"Epub\",\"JCR\":\"Q1\",\"JCRName\":\"MULTIDISCIPLINARY SCIENCES\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences","FirstCategoryId":"103","ListUrlMain":"https://doi.org/10.1098/rsta.2023.0343","RegionNum":3,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2024/12/24 0:00:00","PubModel":"Epub","JCR":"Q1","JCRName":"MULTIDISCIPLINARY SCIENCES","Score":null,"Total":0}
Multiple interacting photonic modes in strongly coupled organic microcavities.
Room-temperature cavity quantum electrodynamics with molecular materials in optical cavities offers exciting prospects for controlling electronic, nuclear and photonic degrees of freedom for applications in physics, chemistry and materials science. However, achieving strong coupling with molecular ensembles typically requires high molecular densities and substantial electromagnetic-field confinement. These conditions usually involve a significant degree of molecular disorder and a highly structured photonic density of states. It remains unclear to what extent these additional complexities modify the usual physical picture of strong coupling developed for atoms and inorganic semiconductors. Using a microscopic quantum description of molecular ensembles in realistic multimode optical resonators, we show that the emergence of vacuum Rabi splitting in linear spectroscopy is a necessary but not sufficient metric of coherent admixing between light and matter. In low-finesse multi-mode situations, we find that molecular dipoles can be partially hybridized with photonic dissipation channels associated with off-resonant cavity modes. These vacuum-induced dissipative processes ultimately limit the extent of light-matter coherence that the system can sustain.This article is part of the theme issue 'The quantum theory of light'.
期刊介绍:
Continuing its long history of influential scientific publishing, Philosophical Transactions A publishes high-quality theme issues on topics of current importance and general interest within the physical, mathematical and engineering sciences, guest-edited by leading authorities and comprising new research, reviews and opinions from prominent researchers.