Transfer of vibrational coherence through incoherent energy transfer process in Forster limit
Transfer of vibrational coherence through incoherent energy transfer process in Forster limit
复制标题
在福斯特极限中通过非相干能量转移过程传递振动相干性
DOI：
10.1139/cjc-2013-0351
复制
发表时间：
2014-02-01
影响因子：
1.1
通讯作者：
Zigmantas, Donatas
中科院分区：
文献类型：
--
作者：
Mancal, Tomas;Dostal, Jakub;Zigmantas, Donatas
我们研究了与非结构化热力学浴和一些明显的振动分子内模式耦合的简单二聚电子系统中激发能量供体和受体之间相干核振荡的转移。我们的重点是这种系统的非线性光学响应，即我们研究激发态能量转移和所谓的基态漂白信号的补偿。响应函数形式使我们能够研究异二聚体，其中单体与浴强烈耦合并通过彼此弱共振耦合（福斯特速率限制）。我们的工作源于最近对能量传输系统二维相干光谱中各种振动特征的观察，其中包括具有快速能量扩散的大型结构。我们发现，只要转移速率足够快，振动相干性就可以从供体分子转移到受体分子。受体分子的基态漂白信号不显示任何振荡特征，并且供体分子的基态漂白信号的振荡以振幅为主，该振幅不随弛豫速率而减小。
We study transfer of coherent nuclear oscillations between an excitation energy donor and an acceptor in a simple dimeric electronic system coupled to an unstructured thermodynamic bath and some pronounced vibrational intramolecular mode. Our focus is on the nonlinear optical response of such a system, i.e., we study both excited state energy transfer and the compensation of the so-called ground-state bleach signal. The response function formalism enables us to investigate a heterodimer with monomers coupled strongly to the bath and by a weak resonance coupling to each other (Forster rate limit). Our work is motivated by recent observation of various vibrational signatures in two-dimensional coherent spectra of energy-transferring systems including large structures with a fast energy diffusion. We find that the vibrational coherence can be transferred from donor to acceptor molecules provided the transfer rate is sufficiently fast. The ground-state bleach signal of the acceptor molecules does not show any oscillatory signatures, and oscillations in ground-state bleaching signal of the donor prevail with the amplitude, which is not decreasing with the relaxation rate.