论文标题
分子极化子的多维相干光谱：langevin方法
Multidimensional Coherent Spectroscopy of Molecular Polaritons: Langevin Approach
论文作者
论文摘要
我们提出了一种微观理论，用于光腔中N分子的非线性光谱。对于时间和频率分辨的信号，量子Langevin分析表达是指任意数量的振动激发的信号。我们从信号的多维投影（例如途径和时间尺度）中确定了极化孔 - 波利龙相互作用的清晰特征。腔体极化子对分子内振动的合作动力学以及远程相干性和振动耦合之间的串扰可能会导致定位效应。我们的结果进一步表征了极化的相干性和较慢的种群转移。
We present a microscopic theory for nonlinear optical spectroscopy of N molecules in an optical cavity. A quantum Langevin analytical expression is derived for the time- and frequency-resolved signals accounting for arbitrary numbers of vibrational excitations. We identify clear signatures of the polariton-polaron interaction from multidimensional projections of the signal, e.g., pathways and timescales. Cooperative dynamics of cavity polaritons against intramolecular vibrations is revealed, along with a cross talk between long-range coherence and vibronic coupling that may lead to localization effects. Our results further characterize the polaritonic coherence and the population transfer that is slower.
