Dodin Amro, Brumer Paul
Chemical Physics Theory Group, Department of Chemistry, and Center for Quantum Information and Quantum Control, University of Toronto, Toronto, Ontario M5S 3H6, Canada.
J Chem Phys. 2019 May 14;150(18):184304. doi: 10.1063/1.5092981.
Dynamics and coherences in retinal isomerization are investigated in a standard two-mode two-state model irradiated by natural incoherent light using the Markovian partial-secular Bloch-Redfield formalism. The two-mode two-state model is a minimal model of retinal that considers vibronic states on a ground and excited electronic manifold coupled to two continuous Ohmic harmonic baths. All light-induced coherent oscillations are shown to disappear as the turn-on time becomes realistically slow. Rather, an interplay between incoherent-light induced coherences and environmentally induced coherences is exposed as the system approaches a nonequilibrium steady state. The dynamics of the system reveal stable steady state coherences under realistic conditions, producing a small but robust transient enhancement of quantum yield.
利用马尔可夫部分久期布洛赫-雷德菲尔德形式理论,在由自然非相干光照射的标准双模二态模型中研究了视网膜异构化中的动力学和相干性。双模二态模型是视网膜的最小模型,它考虑了基态和激发电子流形上的振动状态,这些状态与两个连续的欧姆型谐波浴耦合。随着开启时间变得实际缓慢,所有光诱导的相干振荡都显示会消失。相反,当系统接近非平衡稳态时,非相干光诱导的相干性与环境诱导的相干性之间的相互作用就会显现出来。系统的动力学在实际条件下揭示了稳定的稳态相干性,产生了虽小但稳健的量子产率瞬态增强。