论文标题
光 - 互动中的集体响应：强耦合与局部动力学之间的相互作用
Collective response in light-matter interactions: The interplay between strong coupling and local dynamics
论文作者
论文摘要
研究了一种模型，以模仿分子集合在光腔中的集体光学响应对分子振动动力学的含义。当大量N分子集体响应辐射场时，通常会达到强分子辐射场耦合。在电子强耦合中，偏振子激发之后的分子核动力学反映了（a）一方面快速电子和光子动力学与慢核运动之间的时间尺度分离，以及（b）分子 - 场耦合的集体性质与Molecules核反应对另一个的局部性质的集体性质之间的相互作用。第一个暗示电子激发在近似近似的精神上发生，以大约固定的核构型进行。第二个可以作为一个有趣的问题改造，光激发的集体性质是否会导致北极子形成后的集体核运动，从而导致所谓的极性二极管解耦动力学。 We address this issue by studying the dynamical properties of a simplified Holstein-Tavis-Cummings type model, in which boson modes representing molecular vibrations are replaced by two-level systems while the boson frequency and the vibronic coupling are represented by the coupling between these levels (that induces Rabi oscillations between them) and electronic state dependence of this coupling.我们研究了Polariton激发后这种模型的短时行为及其对CW驱动的响应及其状态频谱的密度。我们发现，尽管动力学行为的某些方面似乎遵守了极化子的脱钩图，但观察到的动力学主要反映了电子极化子的核构型的局部性质，而不是此图片。
A model designed to mimic the implications of the collective optical response of molecular ensembles in optical cavities on molecular vibronic dynamics is investigated. Strong molecule-radiation field coupling is often reached when a large number N of molecules respond collectively to the radiation field. In electronic strong coupling, molecular nuclear dynamics following polariton excitation reflects (a) the timescale separation between the fast electronic and photonic dynamics and the slow nuclear motion on one hand, and (b) the interplay between the collective nature of the molecule-field coupling and the local nature of the molecules nuclear response on the other. The first implies that the electronic excitation takes place, in the spirit of the Born approximation, at an approximately fixed nuclear configuration. The second can be rephrased as the intriguing question, can the collective nature of the optical excitation lead to collective nuclear motion following polariton formation, resulting in so-called polaron decoupled dynamics. We address this issue by studying the dynamical properties of a simplified Holstein-Tavis-Cummings type model, in which boson modes representing molecular vibrations are replaced by two-level systems while the boson frequency and the vibronic coupling are represented by the coupling between these levels (that induces Rabi oscillations between them) and electronic state dependence of this coupling. We investigate the short-time behavior of this model following polariton excitation as well as its response to CW driving and its density of states spectrum. We find that, while some aspects of the dynamical behavior appear to adhere to the polaron decoupling picture, the observed dynamics mostly reflect the local nature of the nuclear configuration of the electronic polariton rather than this picture.
