论文标题
广义共振能量传递理论:光腔中振动能流的应用
Generalized resonance energy transfer theory: Applications to vibrational energy flow in optical cavities
论文作者
论文摘要
共振能量传递的一般速率理论被制定,以结合任何自由度(例如旋转,振动,激子和极化子)以及相干耦合的复合状态。紧凑的速率表达使我们能够建立有用的关系:(i)当捐赠者和受体处于相同温度时的详细平衡条件; (ii)与供体的排放和受体吸收光谱之间重叠的比例; (iii)与有效相干大小的缩放,即相干耦合分子的数量; (iv)从相互作用潜力得出的空间和定向依赖性。当应用于腔体辅助振动能量转移时,速率形式主义提供了对集体振动强耦合方案中的合作,共振和非线性等有趣现象的直观和定量解释,如最近在最近的模拟中所示。
A general rate theory for resonance energy transfer is formulated to incorporate any degrees of freedom (e.g., rotation, vibration, exciton, and polariton) as well as coherently-coupled composite states. The compact rate expression allows us to establish useful relationships: (i) detailed balance condition when the donor and acceptor are at the same temperature; (ii) proportionality to the overlap between donor's emission and acceptor's absorption spectra; (iii) scaling with the effective coherent size, i.e., the number of coherently coupled molecules; (iv) spatial and orientational dependences as derived from the interaction potential. When applied to cavity-assisted vibrational energy transfer, the rate formalism provides an intuitive and quantitative explanation of intriguing phenomena such as cooperativity, resonance, and nonlinearity in the collective vibrational strong coupling regime, as demonstrated in recent simulations.