探索视紫红质与减少视网膜发色团的光动力学。,Journal of Chemical Theory and Computation

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探索视紫红质与减少视网膜发色团的光动力学。
Journal of Chemical Theory and Computation ( IF 5.7 ) Pub Date : 2016-01-06 00:00:00 , DOI: 10.1021/acs.jctc.5b00945
Madushanka Manathunga ₁ , Xuchun Yang ₁ , Hoi Ling Luk ₁ , Samer Gozem ₁ , Luis Manuel Frutos ₂ , Alessio Valentini _{2,

3} , Nicolas Ferrè ₄ , Massimo Olivucci _{1,

3,

5}

Affiliation

尽管已对各种光响应蛋白的光诱导种群动力学进行了光谱研究，但由于合适的高水平量子化学方法的成本过高以及需要传播数百甚至数千种非绝热分子，因此尚未进行系统的计算研究。轨迹。在这里，我们探索通过构建和研究具有减少的视网膜发色团的量子力学/分子力学（QM / MM）模型来研究视紫红质的光动力学的可能性。为此，我们使用在蓝细菌鱼腥藻中发现的感觉视紫红质PCC7120（ASR）作为基准系统。我们发现与ASR QM / MM模型的激发态动力学相关的基本力学特征是使用包含最小（即，三个双键）生色团的模型重现的。此外，我们表明，使用相同的简化模型计算出的非绝热ASR轨迹在CASPT2和CASSCF的理论水平上都可以再现使用非简化模型估算的光谱和寿命趋势，并且可以在室温下通过实验观察到。我们得出的结论是，这些研究的进一步扩展可能会导致低成本QM / MM视紫红质模型，这些模型可用作高通量计算机突变体筛选的有效工具。

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Probing the Photodynamics of Rhodopsins with Reduced Retinal Chromophores

While the light-induced population dynamics of different photoresponsive proteins has been investigated spectroscopically, systematic computational studies have not yet been possible due to the phenomenally high cost of suitable high level quantum chemical methods and the need of propagating hundreds, if not thousands, of nonadiabatic trajectories. Here we explore the possibility of studying the photodynamics of rhodopsins by constructing and investigating quantum mechanics/molecular mechanics (QM/MM) models featuring reduced retinal chromophores. In order to do so we use the sensory rhodopsin found in the cyanobacterium Anabaena PCC7120 (ASR) as a benchmark system. We find that the basic mechanistic features associated with the excited state dynamics of ASR QM/MM models are reproduced using models incorporating a minimal (i.e., three double-bond) chromophore. Furthermore, we show that ensembles of nonadiabatic ASR trajectories computed using the same abridged models replicate, at both the CASPT2 and CASSCF levels of theory, the trends in spectroscopy and lifetimes estimated using unabridged models and observed experimentally at room temperature. We conclude that a further expansion of these studies may lead to low-cost QM/MM rhodopsin models that may be used as effective tools in high-throughput in silico mutant screening.

更新日期：2016-01-06

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