摘要
二维电子光谱(2DES)[1]是飞秒光化学领域最前沿的实验手段之一,它给出全面而直观的光谱动力学信息,可以非常有效地研究超快能量传递与电子转移的动力学过程[2],例如光合作用的原初步骤——将太阳光能转化为电化学能。光合反应中心(RC)色素-蛋白复合物是实现该光电转化的场所,其中多个色素分子形成电子传递链,转化量子效率接近100%。在应用2DES研究了其超高转化率背后的物理机制[3-4]的基础上,我们最近发现了各电荷分离(CT)中间态的存在会影响色素分子周边电场,导致其发生Stark位移。我们阐明了这些信号的物理来源,定量了Stark位移的数值,并分析了Stark信号的衰减动力学。在此基础上,提出了Stark效应对电子转移速率的影响。该工作也证明了2DES中出现的Stark信号可以用来有效地追踪电子转移的动力学过程,适合广泛应用。
Two-dimensional electronic spectroscopy(2 DES)[1]provides a full map of spectral dynamic information and becomes a powerful method to investigate ultrafast energy and electron transfer processes[2].It has been employed to study the physical mechanism behind the high photo-electronic conversion efficiency in reaction center(RC)complex[3-4].We recently find dynamic Stark signals appear in the 2 DES spectra induced by the inherent electric field.The origin and quantitative value of the Stark shift are analyzed,based on which,we proposed that the Stark shift plays a role in modulating the primary charge separation rate.This work demonstrates that Stark signals appearing in 2 DES spectra will help to understand dynamics of electron or charge-transfer intermediate.
作者
马菲
Rienk van Grondelle
于龙江
MA Fei;Rienk van Grondelle;YU Long-jiang(Key Laboratory of Photobiology,Institute of Botany,Chinese Academy of Sciences,Beijing 100093,China;Department of Biophysics,VU University Amsterdam,Amsterdam 1081HV,the Netherlands)
出处
《光谱学与光谱分析》
SCIE
EI
CAS
CSCD
北大核心
2020年第S01期329-330,共2页
Spectroscopy and Spectral Analysis
基金
国家自然科学基金项目(21903086)
国家重点研发项目(2019YFA0904600)资助
