Physical Research Laboratory, Navrangpura, Ahmedabad, 380009, India.
Faraday Discuss. 2011;153:41-50; discussion 73-91. doi: 10.1039/c1fd00038a.
A simple numerical algorithm for solving the non-Markovian master equation in the second Born approximation is developed and used to propagate the traditional dimer system that models electronic energy transfer in photosynthetic systems. Specifically, the coupled integro-differential equations for the reduced density matrix are solved by an efficient auxiliary function method in both the energy and site representations. In addition to giving exact results to this order, the approach allows us to access the range of the reorganization energy and decay rates of the phonon auto-correlation function for which the Markovian Redfield theory and the second-order approximation is useful. For example, the use of Redfield theory for lambda > 10 cm(-1) in Fenna-Mathews-Olson (FMO) type systems is shown to be fundamentally inaccurate.
发展了一种用于求解二级玻恩近似中非马尔可夫主方程的简单数值算法，并将其用于传播传统的二聚体系统，该系统用于模拟光合作用系统中的电子能量转移。具体而言，通过在能量和位置表示中使用有效的辅助函数方法来求解简化密度矩阵的耦合积分微分方程。除了在此阶给出精确结果外，该方法还允许我们访问重组能和声子自相关函数衰减率的范围，对于这些范围，马尔可夫里德理论和二阶近似是有用的。例如，对于 Fenna-Mathews-Olson (FMO) 类型系统中的 lambda > 10 cm(-1)，使用里德理论是根本不准确的。
