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The Effect of Site-Specific Spectral Densities on the High-Dimensional Exciton-Vibrational Dynamics in the FMO Complex
Chemical Physics ( IF 2.3 ) Pub Date : 2017-09-23 , DOI: 10.1016/j.chemphys.2017.09.007
Jan Schulze , Mohamed F. Shibl , Mohammed J. Al-Marri , Oliver Kühn

The coupled exciton-vibrational dynamics of a three-site model of the FMO complex is investigated using the Multi-layer Multi-configuration Time-dependent Hartree (ML-MCTDH) approach. Emphasis is put on the effect of the spectral density on the exciton state populations as well as on the vibrational and vibronic non-equilibrium excitations. Models which use either a single or site-specific spectral densities are contrasted to a spectral density adapted from experiment. For the transfer efficiency, the total integrated Huang-Rhys factor is found to be more important than details of the spectral distributions. However, the latter are relevant for the obtained non-equilibrium vibrational and vibronic distributions and thus influence the actual pattern of population relaxation.

中文翻译:

现场特定光谱密度对FMO复合体中高维激子振动动力学的影响

使用多层多配置时变哈特里(ML-MCTDH)方法研究了FMO复合体三点模型的耦合激子-振动动力学。重点放在频谱密度对激子态种群以及振动和振动非平衡激发的影响上。将使用单个或特定于站点的光谱密度的模型与根据实验改编的光谱密度进行对比。对于传输效率,发现总的综合Rhy-Rhys因子比光谱分布的详细信息更为重要。但是,后者与所获得的非平衡振动和振动分布有关,因此会影响人口松弛的实际模式。
更新日期:2017-09-29
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