Ultrastrong Coupling of a Single Molecule to a Plasmonic Nanocavity: A First-Principles Study.
Journal
ACS photonics
ISSN: 2330-4022
Titre abrégé: ACS Photonics
Pays: United States
ID NLM: 101634366
Informations de publication
Date de publication:
16 Mar 2022
16 Mar 2022
Historique:
received:
12
01
2022
entrez:
21
3
2022
pubmed:
22
3
2022
medline:
22
3
2022
Statut:
ppublish
Résumé
Ultrastrong coupling (USC) is a distinct regime of light-matter interaction in which the coupling strength is comparable to the resonance energy of the cavity or emitter. In the USC regime, common approximations to quantum optical Hamiltonians, such as the rotating wave approximation, break down as the ground state of the coupled system gains photonic character due to admixing of vacuum states with higher excited states, leading to ground-state energy changes. USC is usually achieved by collective coherent coupling of many quantum emitters to a single mode cavity, whereas USC with a single molecule remains challenging. Here, we show by time-dependent density functional theory (TDDFT) calculations that a single organic molecule can reach USC with a plasmonic dimer, consisting of a few hundred atoms. In this context, we discuss the capacity of TDDFT to represent strong coupling and its connection to the quantum optical Hamiltonian. We find that USC leads to appreciable ground-state energy modifications accounting for a non-negligible part of the total interaction energy, comparable to
Identifiants
pubmed: 35308405
doi: 10.1021/acsphotonics.2c00066
pmc: PMC8931765
doi:
Types de publication
Journal Article
Langues
eng
Pagination
1065-1077Informations de copyright
© 2022 The Authors. Published by American Chemical Society.
Déclaration de conflit d'intérêts
The authors declare no competing financial interest.
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