A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä
Ultrastrong Coupling of a Single Molecule to a Plasmonic Nanocavity : A First-Principles Study (2022)

Kuisma, M., Rousseaux, B., Czajkowski, K. M., Rossi, T. P., Shegai, T., Erhart, P., & Antosiewicz, T. J. (2022). Ultrastrong Coupling of a Single Molecule to a Plasmonic Nanocavity : A First-Principles Study. ACS Photonics, 9(3), 1065-1077. https://doi.org/10.1021/acsphotonics.2c00066

JYU-tekijät tai -toimittajat

Julkaisun tiedot

Julkaisun kaikki tekijät tai toimittajat: Kuisma, Mikael; Rousseaux, Benjamin; Czajkowski, Krzysztof M.; Rossi, Tuomas P.; Shegai, Timur; Erhart, Paul; Antosiewicz, Tomasz J.

Lehti tai sarja: ACS Photonics

ISSN: 2330-4022

eISSN: 2330-4022

Julkaisuvuosi: 2022

Ilmestymispäivä: 02.03.2022

Volyymi: 9

Lehden numero: 3

Artikkelin sivunumerot: 1065-1077

Kustantaja: American Chemical Society (ACS)

Julkaisumaa: Yhdysvallat (USA)

Julkaisun kieli: englanti

DOI: https://doi.org/10.1021/acsphotonics.2c00066

Julkaisun avoin saatavuus: Avoimesti saatavilla

Julkaisukanavan avoin saatavuus: Osittain avoin julkaisukanava

Julkaisu on rinnakkaistallennettu (JYX): https://jyx.jyu.fi/handle/123456789/80178

Tiivistelmä

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.

YSO-asiasanat: nanorakenteet; plasmoniikka; fotoniikka; tiheysfunktionaaliteoria

Vapaat asiasanat: strong coupling; time-dependent density functional theory; plasmonics; nanophotonics; excitons

Liittyvät organisaatiot

OKM-raportointi: Kyllä

Raportointivuosi: 2022

JUFO-taso: 2