Molecular emitters located in an optical cavity are known to experience a dramatic modification of the energy and dynamics of their light emission, establishing novel routes for the generation of non-classical states of light. Under monochromatic illumination, spectral asymmetries in cavity-enhanced molecular fluorescence often emerge due to the formation of hybrid polaritonic states (upper and lower polaritons). By applying the theory of open-quantum systems, we show that under strong-coupling conditions, it is essential to account for the interaction of the molecular electronic states with their vibrational environment (dephasing reservoir) to address the complex dynamics of light emission. The interaction with the dephasing reservoir yields a transfer of energy between the polariton states, favoring the transition toward the lower polariton. As a result, we show that the inelastic light emission originates mainly from the lower polariton state regardless of the pumping laser frequency, thus producing asymmetric light emission spectra. Furthermore, we show that, when several molecules are considered, intermolecular coupling can break the symmetry of the system, enabling originally dark polaritons to emit light, as revealed in the fluorescence spectrum by the emergence of new emission peaks. These results stress that accounting for the interaction with dephasing reservoirs is key to interpret molecular light emission in cavities, consistent with experimental observations.

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分子激子-极化子的不对称光发射的起源

已知位于光腔中的分子发射器会经历能量和光发射动力学的显着改变，从而为产生非经典光态建立了新颖的途径。在单色照明下，由于混合极化子状态（上极化子和下极化子）的形成，腔增强分子荧光中的光谱不对称性经常出现。通过应用开放量子系统的理论，我们表明，在强耦合条件下，必须考虑分子电子态与其振动环境（相移储库）的相互作用，以解决复杂的发光动力学问题。与移相储层的相互作用在极化子态之间产生了能量转移，有利于向较低极化子的跃迁。结果表明，无论泵浦激光频率如何，非弹性光发射主要源自较低的极化子态，从而产生不对称的光发射光谱。此外，我们表明，当考虑多个分子时，分子间偶联会破坏系统的对称性，从而使最初的暗极化子能够发光，如荧光光谱中新的发射峰的出现所揭示。这些结果强调，与相移储层的相互作用是解释腔内分子发光的关键，这与实验观察一致。我们表明，当考虑多个分子时，分子间的偶联会破坏系统的对称性，使最初的暗极化子能够发光，如荧光光谱中新的发射峰的出现所揭示。这些结果强调，与相移储层的相互作用是解释腔内分子发光的关键，这与实验观察一致。我们表明，当考虑多个分子时，分子间的偶联会破坏系统的对称性，使最初的暗极化子能够发光，如荧光光谱中新的发射峰的出现所揭示。这些结果强调，与相移储层的相互作用是解释腔内分子发光的关键，这与实验观察一致。