Analytic Model for Molecules Under Collective Vibrational Strong Coupling in Optical Cavities

• URL: http://arxiv.org/abs/2401.16374v1
• Date: Mon, 29 Jan 2024 18:13:43 GMT
• Title: Analytic Model for Molecules Under Collective Vibrational Strong Coupling in Optical Cavities
• Authors: Jacob Horak, Dominik Sidler, Wei-Ming Huang, Michael Ruggenthaler and Angel Rubio
• Abstract summary: We present a model system consisting of an ensemble of N molecules under vibrational strong coupling (VSC) A priori no harmonic approximation is imposed for the inter-nuclear interactions. We highlight that anharmonic intra-molecular interactions might become essential for the formation of local strong coupling effects.
• Score: 0.9824636175880032
• License: http://creativecommons.org/licenses/by/4.0/
• Abstract: Analytical results are presented for a model system consisting of an ensemble of N molecules under vibrational strong coupling (VSC). The single bare molecular model is composed of one effective electron, which couples harmonically to multiple nuclei. A priori no harmonic approximation is imposed for the inter-nuclear interactions. Within the cavity Born-Oppenheimer partitioning, i.e., when assuming classical nuclei and displacement field coordinates, the dressed N-electron problem can be solved analytically in the dilute limit. In more detail, we present a self-consistent solution of the corresponding cavity-Hartree equations, which illustrates the relevance of the non-perturbative treatment of electronic screening effects under VSC. We exemplify our derivations for an ensemble of harmonic model CO2 molecules, which shows that common simplifications can introduce non-physical effects (e.g., a spurious coupling of the transverse field to the center-of-mass motion for neutral atoms). In addition, our self-consistent solution reveals a simple analytic expression for the cavity-induced red shift and the associated refractive index, which can be interpreted as a polarizability-dependent detuning of the cavity. Finally, we highlight that anharmonic intra-molecular interactions might become essential for the formation of local strong coupling effects within a molecular ensemble under collective VSC.

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