模型视网膜稳态光致异构的极端参数敏感性
Extreme Parametric Sensitivity in the Steady-State Photoisomerization of Model Retinal
摘要：
利用热浴耦合的两态双模模型对视紫红质中的视黄质发色团的光异构化反应进行了计算研究。在稳态（10 ps及以上）的反应量子产率被发现是显着不同的瞬态值，这表明在这些系统中的瞬态和稳态动力学之间的弱相关性。值得注意的是，稳态量子产率对系统参数的微小变化非常敏感，而瞬态动力学几乎不受影响。这种灵敏度与非绝热电子振动系统的标准能级间距统计的相关性表明量子混沌可能起源于此。讨论了实验观测这一现象的可行性及其在凝聚相光化学和生物光传感中的意义。
英文摘要：
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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