论文标题

模型视网膜的稳态光异构化中的极端参数灵敏度

Extreme Parametric Sensitivity in the Steady-State Photoisomerization of Model Retinal

论文作者

Chuang, Chern, Brumer, Paul

论文摘要

使用与热浴的两态两种模型模型对视网膜蛋白中视网膜生色团的光异构化反应进行了计算研究。发现在稳态(10 ps及以上)处的反应量子产率与它们的瞬态值有很大不同,这表明在这些系统中瞬时和稳态动力学之间存在弱相关性。值得注意的是,稳态量子产率对系统参数的微小变化高度敏感,而瞬态动力学几乎不受影响。这种敏感性与非绝热振动系统的标准水平间距统计数据的相关性表明量子混乱中可能存在起源。讨论了对这种现象的实验观察的可行性及其在凝聚相光化学和生物光感应中的影响。

The photoisomerization reaction of the retinal chromophore in rhodopsin was computationally studied using a two-state two-mode model coupled to thermal baths. Reaction quantum yields at the steady state (10 ps and beyond) were found to be considerably different than their transient values, suggesting a weak correlation between transient and steady-state dynamics in these systems. Significantly, the steady-state quantum yield was highly sensitive to minute changes in system parameters, while transient dynamics was nearly unaffected. Correlation of such sensitivity with standard level spacing statistics of the nonadiabatic vibronic system suggests a possible origin in quantum chaos. The feasibility of experimental observation of this phenomenon and its implications in condensed-phase photochemistry and biological light sensing are discussed.

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