Quantum theory of collective strong coupling of molecular vibrations with a microcavity mode

We develop a quantum mechanical formalism to treat the strong coupling between an electromagnetic mode and a vibrational excitation of an ensemble of organic molecules. By employing a Bloch-Redfield-Wangsness approach, we show that the influence of dephasing-type interactions, i.e., elastic collisio...

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Detalles Bibliográficos
Autores: Pino, Javier del, Feist, Johannes, García Vidal, Fco. José
Tipo de recurso: artículo
Fecha de publicación:2015
País:España
Institución:Universidad Autónoma de Madrid
Repositorio:Biblos-e Archivo. Repositorio Institucional de la UAM
Idioma:inglés
OAI Identifier:oai:repositorio.uam.es:10486/676139
Acceso en línea:http://hdl.handle.net/10486/676139
https://dx.doi.org/10.1088/1367-2630/17/5/053040
Access Level:acceso abierto
Palabra clave:Organic molecules
Strong coupling
Vibrational modes
Polaritons
Quantum optics
Física
Descripción
Sumario:We develop a quantum mechanical formalism to treat the strong coupling between an electromagnetic mode and a vibrational excitation of an ensemble of organic molecules. By employing a Bloch-Redfield-Wangsness approach, we show that the influence of dephasing-type interactions, i.e., elastic collisions with a background bath of phonons, critically depends on the nature of the bath modes. In particular, for long-range phonons corresponding to a common bath, the dynamics of the 'bright state' (the collective superposition of molecular vibrations coupling to the cavity mode) is effectively decoupled from other system eigenStates. For the case of independent baths (or short-range phonons), incoherent energy transfer occurs between the bright state and the uncoupled dark States. However, these processes are suppressed when the Rabi splitting is larger than the frequency range of the bath modes, as achieved in a recent experiment (Shalabney et al 2015 Nat. Commun. 6 5981). In both cases, the dynamics can thus be described through a single collective oscillator coupled to a photonic mode, making this system an ideal candidate to explore cavity optomechanics at room temperature