论文标题
模型视紫红蛋白的稳态光异构化量子产率：波袋动力学的见解？
Steady State Photoisomerization Quantum Yield of Model Rhodopsin: Insights from Wavepacket Dynamics?
论文作者
论文摘要
我们基于耦合到热环境的两态二摩德模型，模拟了视网膜蛋白中的视网膜色素的非平衡稳态\ textit {cis-trans}光异构化。通过分析系统不均匀扩大整体内部的系统趋势，我们发现稳态反应量子产率（QY）与系统交叉点以上的过量能量密切相关，与短时间动态波动板图的预测一致。但是，QY对系统环境相互作用的非平地依赖性表明纯动力学图像不足，环境诱导的部分内部能量重新分布发生在反应结束之前。这些结果表明，对光异构化反应的适当处理，尤其是其高QY，必须解释能量的重新分布和耗散，而不是在文献中通常使用的动态波袋运动以外的动态波袋运动，并且仅在短暂性方面是适当的。
We simulate the nonequilibrium steady state \textit{cis-trans} photoisomerization of retinal chromophore in rhodopsin based on a two-state-two-mode model coupled to a thermal environment. By analyzing the systematic trends within an inhomogeneously broadened ensemble of systems, we find that the steady state reaction quantum yield (QY) correlates strongly with the excess energy above the crossing point of the system, in agreement with the prediction of the short time dynamical wavepacket picture. However, the nontrivial dependence of the QY on the system-environment interaction indicates that a pure dynamical picture is insufficient and that environment-induced partial internal energy redistribution takes place before the reaction concludes. These results imply that a proper treatment of the photoisomerization reaction, particularly its high QY, must account for the redistribution and dissipation of energy beyond the dynamical wavepacket motion that is typically employed in the literature and that is appropriate only in the transient regime.
