论文标题
从混合层次层次方程进行的耦合电荷和能量传递动力学在运动方法中
Coupled charge and energy transfer dynamics in light harvesting complexes from a hybrid hierarchical equations of motion approach
论文作者
论文摘要
我们描述了一种模拟蛋白质色素复合物中激子动力学的方法，包括电荷转移和荧光的效果。该方法结合了运动的层次方程，用于描述激子的量子动力学和Nakajima-Zwanzig量子量子大师方程，该方程用于描述较慢的电荷传输过程。我们研究了在光收集复合物II中的电荷转移淬灭II，这是一种蛋白质，该蛋白质用于控制许多植物物种中的非光化淬灭。使用我们的混合方法，我们发现我们的计算与激发寿命的实验测量之间有很好的一致性。此外，我们的计算表明，激子能量漏斗在确定淬火效率方面起着重要作用，这一结论我们希望扩展到其他执行保护性激发猝灭的蛋白质。这也强调了对正确说明激子动态和电荷传输过程相互作用的仿真方法的需求。
We describe a method for simulating exciton dynamics in protein-pigment complexes, including effects from charge transfer as well as fluorescence. The method combines the hierarchical equations of motion, which are used to describe quantum dynamics of excitons, and the Nakajima-Zwanzig quantum master equation, which is used to describe slower charge transfer processes. We study the charge transfer quenching in light harvesting complex II, a protein postulated to control non-photochemcial quenching in many plant species. Using our hybrid approach, we find good agreement between our calculation and experimental measurements of the excitation lifetime. Furthermore our calculations reveal that the exciton energy funnel plays an important role in determining quenching efficiency, a conclusion we expect to extend to other proteins that perform protective excitation quenching. This also highlights the need for simulation methods that properly account for the interplay of exciton dynamics and charge transfer processes.
