Department of Chemistry and Birck Nanotechnology Center, Purdue University, West Lafayette, Indiana 47907, USA.
J Phys Chem B. 2011 Feb 17;115(6):1531-7. doi: 10.1021/jp109559p. Epub 2011 Jan 26.
We present a detailed theoretical study of the transfer of electronic excitation energy through the Fenna-Matthews-Olson (FMO) pigment-protein complex, using the newly developed modified scaled hierarchical approach (Shi, Q.; et al. J. Chem. Phys. 2009, 130, 084105). We show that this approach is computationally more efficient than the original hierarchical approach. The modified approach reduces the truncation levels of the auxiliary density operators and the correlation function. We provide a systematic study of how the number of auxiliary density operators and the higher-order correlation functions affect the exciton dynamics. The time scales of the coherent beating are consistent with experimental observations. Furthermore, our theoretical results exhibit population beating at physiological temperature. Additionally, the method does not require a low-temperature correction to obtain the correct thermal equilibrium at long times.
我们使用新开发的改进的缩放分层方法（Shi，Q.；等。J. Chem. Phys. 2009，130，084105）对通过 Fenna-Matthews-Olson（FMO）色素蛋白复合物传递电子激发能进行了详细的理论研究。我们表明，该方法在计算上比原始分层方法更有效。改进的方法减少了辅助密度算符和相关函数的截断水平。我们系统地研究了辅助密度算符的数量和高阶相关函数如何影响激子动力学。相干拍频的时间尺度与实验观察一致。此外，我们的理论结果在生理温度下表现出了种群拍频。此外，该方法不需要低温修正即可在长时间内获得正确的热平衡。
