Ultrastrong Coupling of a Single Molecule to a Plasmonic Nanocavity: A First-Principles Study
Artikel i vetenskaplig tidskrift, 2022

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.

nanophotonics

plasmonics

time-dependent density functional theory

strong coupling

excitons

Författare

Mikael Juhani Kuisma

Jyväskylän Yliopisto

Chalmers, Fysik, Material- och ytteori

Benjamin Rousseaux

Ecole Normale Superieure (ENS)

Chalmers, Mikroteknologi och nanovetenskap, Tillämpad kvantfysik

K. M. Czajkowski

Uniwersytet Warszawski

Tuomas Rossi

Aalto-Yliopisto

Chalmers, Fysik, Kondenserad materie- och materialteori

Timur Shegai

Chalmers, Fysik, Nano- och biofysik

Paul Erhart

Chalmers, Fysik, Kondenserad materie- och materialteori

Tomasz Antosiewicz

Uniwersytet Warszawski

Chalmers, Fysik, Bionanofotonik

ACS Photonics

2330-4022 (eISSN)

Vol. In Press

Towards nanoscale reality in plasmonic hot-carrier generation (RealNanoPlasmon)

Europeiska kommissionen (EU) (EC/H2020/838996), 2019-04-01 -- 2021-03-31.

Plasmon-exciton coupling at the attosecond-subnanometer scale: Tailoring strong light-matter interactions at room temperature

Knut och Alice Wallenbergs Stiftelse (2019.0140), 2020-07-01 -- 2025-06-30.

Kvantplasmonik – en teknologi för foton-fotonväxelverkan på kvantnivå vid rumstemperatur

Vetenskapsrådet (VR) (2016-06059), 2017-01-01 -- 2022-12-31.

Ämneskategorier

Atom- och molekylfysik och optik

Annan fysik

Den kondenserade materiens fysik

DOI

10.1021/acsphotonics.2c00066

PubMed

35308405

Mer information

Senast uppdaterat

2022-04-07