School of Engineering and Science, Jacobs University Bremen, Campus Ring 1, 28759 Bremen, Germany.
J Phys Chem B. 2013 Jun 20;117(24):7157-63. doi: 10.1021/jp311380k. Epub 2013 Jun 6.
Experimental findings of long-lived quantum coherence in the Fenna-Matthews-Olson (FMO) complex and other photosynthetic complexes have led to theoretical studies searching for an explanation of this unexpected phenomenon. Extending in this regard our own earlier calculations, we performed simulations of the FMO complex in a glycerol-water mixture at 310 K as well as 77 K, matching the conditions of earlier 2D spectroscopic experiments by Engel et al. The calculations, based on an improved quantum procedure employed by us already, yielded spectral densities of each individual pigment of FMO, in water and glycerol-water solvents at ambient temperature that compare well to prior experimental estimates. Due to the slow solvent dynamics at 77 K, the present results strongly indicate the presence of static disorder, i.e., disorder on a time scale beyond that relevant for the construction of spectral densities.
在 Fenna-Matthews-Olson (FMO) 复合物和其他光合复合物中观察到长寿命量子相干的实验结果，促使理论研究寻求对此意外现象的解释。在这方面扩展我们自己之前的计算，我们在 310 K 和 77 K 下模拟了甘油-水混合物中的 FMO 复合物，与 Engel 等人之前的 2D 光谱实验条件相匹配。基于我们已经使用的改进量子程序的计算，得出了 FMO 中每个单独色素在水和甘油-水溶剂中的光谱密度，与之前的实验估计值非常吻合。由于 77 K 时溶剂动力学较慢，目前的结果强烈表明存在静态无序，即在与光谱密度构建相关的时间尺度之外存在无序。
