Fidler Andrew F, Singh Ved P, Long Phillip D, Dahlberg Peter D, Engel Gregory S
Department of Chemistry, The James Franck Institute and The Institute for Biophysical Dynamics, The University of Chicago, Chicago, Illinois 60637, USA.
J Phys Chem Lett. 2013 May 2;4(9):1404-1409. doi: 10.1021/jz400438m.
The initial dynamics of energy transfer in the light harvesting complex 2 from were investigated with polarization controlled two-dimensional spectroscopy. This method allows only the coherent electronic motions to be observed revealing the timescale of dephasing among the excited states. We observe persistent coherence among all states and assign ensemble dephasing rates for the various coherences. A simple model is utilized to connect the spectroscopic transitions to the molecular structure, allowing us to distinguish coherences between the two rings of chromophores and coherences within the rings. We also compare dephasing rates between excited states to dephasing rates between the ground and excited states, revealing that the coherences between excited states dephase on a slower timescale than coherences between the ground and excited states.
利用偏振控制二维光谱研究了来自[具体来源未给出]的光捕获复合物2中能量转移的初始动力学。该方法仅允许观察相干电子运动,从而揭示激发态之间的退相时间尺度。我们观察到所有状态之间存在持续的相干性,并为各种相干性确定了系综退相速率。利用一个简单模型将光谱跃迁与分子结构联系起来,使我们能够区分发色团两个环之间的相干性以及环内的相干性。我们还比较了激发态之间的退相速率与基态和激发态之间的退相速率,结果表明激发态之间的相干性在比基态和激发态之间的相干性更慢的时间尺度上退相。