Physical review. A/Physical review, A · 2016 · 119 citations · 56 references
Natural SciencesChemistryPhysicsMolecular PhysicsOpticsSpectroscopyInfrared SpectroscopyMolecular SpectroscopyNonlinear OpticsOptical SpectroscopyRotational SpectroscopyRotational StructureAbsorption SpectrumExciton-polariton CouplingMolecular Quantum StatesOptical Absorption SpectraPolariton PhysicsSpectral FeaturesStrong Light-matter CouplingTemperature Dependence
Starting from a microscopic model, we investigate the optical spectra of molecules in strongly coupled organic microcavities examining how they might self-consistently adapt their coupling to light. We consider both rotational and vibrational degrees of freedom, focusing on features which can be seen in the peak in the center of the spectrum at the bare excitonic frequency. In both cases we find that the matter-light coupling can lead to a self-consistent change of the molecular states, with consequent temperature-dependent signatures in the absorption spectrum. However, for typical parameters, these effects are much too weak to explain recent measurements. We show that another mechanism which naturally arises from our model of vibrationally dressed polaritons has the right magnitude and temperature dependence to be at the origin of the observed data.
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Coherence in Spontaneous Radiation Processes
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