论文标题
密集介质无序的合奏中的分子极化学
Molecular polaritonics in dense mesoscopic disordered ensembles
论文作者
论文摘要
我们研究了真空狂犬分裂（VRS）对频率障碍，振动，近场效应和分子偏光层密度的依赖性。在介观极限中，仅静态频率障碍已经可以将极化状态的损失机制引入到一个黑暗状态储层中，我们对此进行了定量描述，从而提供了VRS的分析缩放，并具有障碍的水平。障碍还可以将分子集合分成供体类型和受体型分子，以及振动耦合，偶极 - 偶极相互作用和振动弛豫的组合，可引起集体分子状态内兴奋的不一致的FRET（Försterresonance Resonance Enmenance Enmenance Enmenance转移）。这等同于耗散障碍，具有饱和的效果，甚至降低了介质高密度极限中的VR。总体而言，该分析允许量化黑色状态在腔量子量子动力学中所起的关键作用，并具有介观，无序的合奏。
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.
