Computational elucidations on the role of vibrations in energy transfer processes of photosynthetic complexes,Physical Chemistry Chemical Physics

当前位置： X-MOL 学术 › Phys. Chem. Chem. Phys. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

Computational elucidations on the role of vibrations in energy transfer processes of photosynthetic complexes
Physical Chemistry Chemical Physics ( IF 2.9 ) Pub Date : 2021-11-26 , DOI: 10.1039/d1cp04615b
Kwang Hyun Cho ₁ , Young Min Rhee ₁

Affiliation

Coupling between pigment excitations and nuclear movements in photosynthetic complexes is known to modulate the excitation energy transfer (EET) efficiencies. Toward providing microscopic information, researchers often apply simulation techniques and investigate how vibrations are involved in EET processes. Here, reports on such roles of nuclear movements are discussed from a theory perspective. While vibrations naturally present random thermal fluctuations that can affect energy transferring characteristics, they can also be intertwined with exciton structures and create more specific non-adiabatic energy transfer pathways. For reliable simulations, a bath model that accurately mimics a given molecular system is required. Methods for obtaining such a model in combination with quantum chemical electronic structure calculations and molecular dynamics trajectory simulations are discussed. Various quantum dynamics simulation tools that can handle pigment-to-pigment energy transfers together with their vibrational characters are also touched on. Behaviors of molecular vibrations often deviate from ideality, especially when all-atom details are included, which practically forces us to treat them classically. We conclude this perspective by considering some recent reports that suggest that classical descriptions of bath effects with all-atom details may still produce valuable information for analyzing sophisticated contributions by vibrations to EET processes.

中文翻译：

振动在光合复合物能量转移过程中作用的计算阐明

已知光合复合物中色素激发和核运动之间的耦合可调节激发能量转移 (EET) 效率。为了提供微观信息，研究人员经常应用模拟技术并研究振动如何参与 EET 过程。在这里，从理论的角度讨论了关于核运动的这种作用的报告。虽然振动自然会呈现随机的热波动，这会影响能量传递特性，但它们也可以与激子结构交织在一起，并产生更具体的非绝热能量传递路径。为了进行可靠的模拟，需要一个准确模拟给定分子系统的浴模型。讨论了结合量子化学电子结构计算和分子动力学轨迹模拟来获得这种模型的方法。还涉及了可以处理颜料到颜料的能量转移及其振动特性的各种量子动力学模拟工具。分子振动的行为经常偏离理想状态，尤其是当包括全原子细节时，这实际上迫使我们以经典方式对待它们。我们通过考虑最近的一些报告来总结这一观点，这些报告表明，具有全原子细节的浴效应的经典描述仍然可以为分析振动对 EET 过程的复杂贡献提供有价值的信息。还涉及了可以处理颜料到颜料的能量转移及其振动特性的各种量子动力学模拟工具。分子振动的行为经常偏离理想状态，尤其是当包括全原子细节时，这实际上迫使我们以经典方式对待它们。我们通过考虑最近的一些报告来总结这一观点，这些报告表明，具有全原子细节的浴效应的经典描述仍然可以为分析振动对 EET 过程的复杂贡献提供有价值的信息。还涉及了可以处理颜料到颜料的能量转移及其振动特性的各种量子动力学模拟工具。分子振动的行为经常偏离理想状态，尤其是当包括全原子细节时，这实际上迫使我们以经典方式对待它们。我们通过考虑最近的一些报告来总结这一观点，这些报告表明，具有全原子细节的浴效应的经典描述仍然可以为分析振动对 EET 过程的复杂贡献提供有价值的信息。

更新日期：2021-11-30

点击分享查看原文

点击收藏

阅读更多本刊最新论文本刊介绍/投稿指南11