Abramavicius Darius, Valkunas Leonas
Department of Theoretical Physics, Vilnius University, Sauletekio al. 9-III, 10222, Vilnius, Lithuania.
Center for Physical Sciences and Technology, A. Gostauto 11, 01108, Vilnius, Lithuania.
Photosynth Res. 2016 Jan;127(1):33-47. doi: 10.1007/s11120-015-0080-6. Epub 2015 Jan 25.
Oscillatory features of two-dimensional spectra of photosynthetic pigment-protein complexes during few picoseconds after electronic excitations of chlorophylls in various pigment-proteins were recently related to the coherent nuclear vibrations. It has been also speculated that the vibrations may assist the excitonic energy transfer and charge separation, hence contributing to energy transport and energy conversion efficiency. Here, we consider three theoretical approaches usually used for characterization of the excitation dynamics and charge separation, namely Redfield, Förster, and Marcus model descriptions, regarding this question. We show that two out of the three mechanisms require explicit resonances of excitonic splittings and the nuclear vibration frequencies. However, the third one related to the electron transfer is in principle off resonant.
最近，在各种色素蛋白中叶绿素发生电子激发后的几皮秒内，光合色素蛋白复合物二维光谱的振荡特征与相干核振动有关。也有人推测，这些振动可能有助于激子能量转移和电荷分离，从而提高能量传输和能量转换效率。在此，我们针对这个问题考虑三种通常用于表征激发动力学和电荷分离的理论方法，即雷德菲尔德（Redfield）、福斯特（Förster）和马库斯（Marcus）模型描述。我们表明，这三种机制中的两种需要激子分裂和核振动频率的明确共振。然而，与电子转移相关的第三种机制原则上是非共振的。
