DISAFA, University of Torino, Grugliasco, I-10095, Italy.
Department of Theoretical Chemistry, Technische Universität München, Garching, D-85747, Germany.
Sci Rep. 2017 Aug 22;7(1):9127. doi: 10.1038/s41598-017-08901-2.
Quantum electron-vibrational dynamics in molecular systems at finite temperature is described using an approach based on Thermo Field Dynamics theory. This formulation treats temperature effects in the Hilbert space without introducing the Liouville space. The solution of Thermo Field Dynamics equations with a novel technique for the propagation of Tensor Trains (Matrix Product States) is implemented and discussed. The methodology is applied to the study of the exciton dynamics in the Fenna-Mathews-Olsen complex using a realistic structured spectral density to model the electron-phonon interaction. The results of the simulations highlight the effect of specific vibrational modes on the exciton dynamics and energy transfer process, as well as call for careful modeling of electron-phonon couplings.
本文采用基于热力学场动力学理论的方法描述了有限温度下分子体系中的量子电子-振动动力学。这种方法在不引入刘维尔空间的情况下，在希尔伯特空间中处理温度效应。利用张量网络（矩阵乘积态）传播的新技术实现并讨论了热力学场动力学方程的解。该方法应用于芬纳-马修斯-奥尔森复合物中激子动力学的研究，使用现实的结构化光谱密度来模拟电子-声子相互作用。模拟结果突出了特定振动模式对激子动力学和能量转移过程的影响，同时也呼吁对电子-声子耦合进行仔细建模。
