Tensor Network Path Integral Study of Dynamics in B850 LH2 Ring with Atomistically Derived Vibrations
Tensor Network Path Integral Study of Dynamics in B850 LH2 Ring with Atomistically Derived Vibrations
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DOI：
10.1021/acs.jctc.2c00163
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发表时间：
2022-06-22
影响因子：
5.5
通讯作者：
Walters, Peter L.
中科院分区：
文献类型：
--
作者：
Bose, Amartya;Walters, Peter L.
最近引入的多站点张量网络路径积分（MS-TNPI）允许模拟耦合到耗散介质的扩展量子系统。利用MS-TNPI模拟了B850细菌叶绿素（BChl）环的激子输运和吸收光谱。对MS-TNPI网络进行了扩展，以适应B850系统的环形拓扑结构。通过Feynman-Vernon影响泛函的框架，将分子振动和蛋白质支架的精确的基于分子动力学的描述结合起来。为了将本工作与激子图像联系起来，通过使用近似和拓扑一致的跃迁偶极矩矢量来模拟吸收谱，从而对吸收谱进行了探索。这些数值精确的MS-TNPI吸收光谱的比较显示与二阶累积量近似。温度对精确谱和近似谱的影响也进行了探讨。
The recently introduced multisite tensor network path integral (MS-TNPI) allows simulation of extended quantum systems coupled to dissipative media. We use MS-TNPI to simulate the exciton transport and the absorption spectrum of a B850 bacteriochlorophyll (BChl) ring. The MS-TNPI network is extended to account for the ring topology of the B850 system. Accurate molecular-dynamics-based description of the molecular vibrations and the protein scaffold is incorporated through the framework of Feynman-Vernon influence functional. To relate the present work with the excitonic picture, an exploration of the absorption spectrum is done by simulating it using approximate and topologically consistent transition dipole moment vectors. Comparison of these numerically exact MS-TNPI absorption spectra are shown with second-order cumulant approximations. The effect of temperature on both the exact and the approximate spectra is also explored.