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Strong plasmon-molecule coupling at the nanoscale revealed by first-principles modeling

dc.abstract.enStrong light-matter interactions in both the single-emitter and collective strong coupling regimes attract significant attention due to emerging applications in quantum and nonlinear optics as well as opportunities for modifying material-related properties. Exploration of these phenomena is theoretically demanding, as polaritons exist at the intersection between quantum optics, solid state physics, and quantum chemistry. Fortunately, nanoscale polaritons can be realized in small plasmon-molecule systems, enabling treatment with ab initio methods. Here, we show that time-dependent density-functional theory calculations access the physics of nanoscale plasmon-molecule hybrids and predict vacuum Rabi splitting. By considering a system comprising a few-hundred-atom aluminum nanoparticle interacting with benzene molecules, we show that cavity quantum electrodynamics holds down to resonators of a few cubic nanometers in size, yielding a single-molecule coupling strength exceeding 200 meV due to a massive vacuum field of 4.5 V · nm−1. In a broader perspective, ab initio methods enable parameter-free in-depth studies of polaritonic systems for emerging applications.
dc.affiliationUniwersytet Warszawski
dc.contributor.authorAntosiewicz, Tomasz
dc.date.accessioned2024-01-26T08:21:00Z
dc.date.available2024-01-26T08:21:00Z
dc.date.issued2019
dc.description.financeNie dotyczy
dc.description.volume10
dc.identifier.doi10.1038/S41467-019-11315-5
dc.identifier.issn2041-1723
dc.identifier.urihttps://repozytorium.uw.edu.pl//handle/item/120858
dc.identifier.weblinkhttps://www.nature.com/articles/s41467-019-11315-5#article-info
dc.languageeng
dc.pbn.affiliationphysical sciences
dc.relation.ispartofNature Communications
dc.relation.pagesart. 3336
dc.rightsClosedAccess
dc.sciencecloudnosend
dc.titleStrong plasmon-molecule coupling at the nanoscale revealed by first-principles modeling
dc.typeJournalArticle
dspace.entity.typePublication