Abstract
Strong light-matter interactions facilitate not only emerging applications in quantum and non-linear optics but also modifications of properties of materials. In particular, the latter possibility has spurred the development of advanced theoretical techniques that can accurately capture both quantum optical and quantum chemical degrees of freedom. These methods are, however, computationally very demanding, which limits their application range. Here, we demonstrate that the optical spectra of nanoparticle-molecule assemblies, including strong coupling effects, can be predicted with good accuracy using a subsystem approach, in which the response functions of different units are coupled only at the dipolar level. We demonstrate this approach by comparison with previous time-dependent density functional theory calculations for fully coupled systems of Al nanoparticles and benzene molecules. While the present study only considers few-particle systems, the approach can be readily extended to much larger systems and to include explicit optical-cavity modes.
Highlights
The coupling of light and matter in the strong coupling (SC) regime leads to the emergence of excited states of mixed nature,1 which are characterized by a coherent energy exchange between the subsystems at a rate that is much faster than the respective damping rates
We have recently demonstrated the usefulness of density functional theory (DFT)30,31 and time-dependent DFT (TDDFT)32 calculations for studying polariton physics in NP–molecule scitation.org/journal/jcp systems
We have analyzed the efficacy of the dipolar coupling (DC) approximation for capturing the emergence of SC in Al NP–benzene hybrid systems
Summary
The coupling of light and matter in the strong coupling (SC) regime leads to the emergence of excited states of mixed nature, which are characterized by a coherent energy exchange between the subsystems at a rate that is much faster than the respective damping rates. Emitter and the cavity form a light–matter hybrid (polariton) with modified and tunable properties, including nonlinear and quantum optical phenomena, photochemical rates, thermally activated ground-state chemical reactions under vibrational SC, and exciton transport.. Emitter and the cavity form a light–matter hybrid (polariton) with modified and tunable properties, including nonlinear and quantum optical phenomena, photochemical rates, thermally activated ground-state chemical reactions under vibrational SC, and exciton transport.18,19 Theoretical analysis of these phenomena is non-trivial as polaritons reside at the intersection between quantum optics, quantum chemistry, and solid state physics. While quantum optical approaches such as Jaynes–Cummings or Dicke models have been used extensively, they are ill-suited for describing the material aspects This has spurred the development of advanced theoretical techniques in recent years based on various quantum optical and quantum chemistry methods.. Ensemble effects and the collective interaction of molecules and/or nanoparticles (NPs) are of immediate experimental interest, calling for methods that allow one to bridge between system specific predictions and computational efficiency
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