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

Kuisma, Mikael Juhani,1984Jyväskylän Yliopisto,University of Jyväskylä,Chalmers tekniska högskola,Chalmers University of Technology (författare)

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.

Rousseaux, Benjamin,1988Ecole Normale Superieure (ENS),Sorbonne Université,Sorbonne University(Swepub:cth)benrou (författare)
Czajkowski, K. M.Uniwersytet Warszawski,University of Warsaw (författare)
Rossi, Tuomas,1988Aalto-Yliopisto,Aalto University,Chalmers tekniska högskola,Chalmers University of Technology(Swepub:cth)rtuomas (författare)
Shegai, Timur,1982Chalmers tekniska högskola,Chalmers University of Technology(Swepub:cth)timurs (författare)
Erhart, Paul,1978Chalmers tekniska högskola,Chalmers University of Technology(Swepub:cth)erhart (författare)
Antosiewicz, Tomasz,1981Chalmers tekniska högskola,Chalmers University of Technology,Uniwersytet Warszawski,University of Warsaw(Swepub:cth)tomasza (författare)
Jyväskylän YliopistoChalmers tekniska högskola (creator_code:org_t)

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