Ultrastrong Coupling of a Single Molecule to a Plasmonic Nanocavity: A First-Principles Study

Mikael Kuisma, Benjamin Rousseaux, Krzysztof M. Czajkowski, Tuomas P. Rossi, Timur Shegai, Paul Erhart, Tomasz J. Antosiewicz*

*Tämän työn vastaava kirjoittaja

Tutkimustuotos: LehtiartikkeliArticleScientificvertaisarvioitu

1 Sitaatiot (Scopus)
8 Lataukset (Pure)

Abstrakti

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 kBT at room temperature.

AlkuperäiskieliEnglanti
Sivut1065-1077
Sivumäärä13
JulkaisuACS Photonics
Vuosikerta9
Numero3
Varhainen verkossa julkaisun päivämäärä2022
DOI - pysyväislinkit
TilaJulkaistu - 16 maalisk. 2022
OKM-julkaisutyyppiA1 Julkaistu artikkeli, soviteltu

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