稠密介观无序系综中的分子极化激元
Molecular polaritonics in dense mesoscopic disordered ensembles
摘要：
本文研究了分子极化激元学中真空拉比分裂（VRS）与频率无序、振动、近场效应和密度的关系。在介观极限，静态频率无序已经可以引入一个损失机制，从极化激元状态到暗态水库，我们定量描述，提供了一个分析缩放的VRS与无序的水平。无序还可以将分子系综分裂成供体型和受体型分子，并且电子振动耦合、偶极-偶极相互作用和振动弛豫的组合诱导集体分子状态内的激发的非相干FRET（Förster共振能量转移）迁移。这相当于一个耗散无序，并具有饱和的效果，甚至减少了介观，高密度极限的VRS。总的来说，这种分析可以量化暗态在腔量子电动力学与介观，无序合奏发挥的关键作用。
英文摘要：
We study the dependence of the vacuum Rabi splitting (VRS) on frequency disorder, vibrations, near-field effects and density in molecular polaritonics. In the mesoscopic limit, static frequency disorder alone can already introduce a loss mechanism from polaritonic states into a dark state reservoir, which we quantitatively describe, providing an analytical scaling of the VRS with the level of disorder. Disorder additionally can split a molecular ensemble into donor-type and acceptor-type molecules and the combination of vibronic coupling, dipole-dipole interactions and vibrational relaxation induces an incoherent FRET (Förster resonance energy transfer) migration of excitations within the collective molecular state. This is equivalent to a dissipative disorder and has the effect of saturating and even reducing the VRS in the mesoscopic, high-density limit. Overall, this analysis allows to quantify the crucial role played by dark states in cavity quantum electrodynamics with mesoscopic, disordered ensembles.
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