Palmieri Benoit, Abramavicius Darius, Mukamel Shaul
Department of Chemistry, University of California, Irvine, California 92697-2025, USA.
J Chem Phys. 2009 May 28;130(20):204512. doi: 10.1063/1.3142485.
Recent experimental observations of time-resolved multidimensional signals in the light-harvesting antennae Fenna-Mathews-Olson [G. S. Engel et al., Nature (London) 446, 782 (2007)] show large oscillations of exciton populations coupled to the long-lived coherences. These effects may not be reproduced by the standard Redfield theory which assumes weak coupling to a bath. A more general relaxation superoperator which holds for all system-bath coupling parameter regimes is constructed by taking into account the statistics (covariances) of Lindblad equation parameters. Simulations for a model dimer reproduce all observed strong coupling effects.
近期对光捕获天线芬纳 - 马修斯 - 奥尔森中时间分辨多维信号的实验观测[G. S. 恩格尔等人,《自然》(伦敦)446, 782 (2007)]表明,与长寿命相干性耦合的激子布居存在大幅振荡。这些效应可能无法由假设与热库弱耦合的标准雷德菲尔德理论再现。通过考虑林德布拉德方程参数的统计量(协方差),构建了一个适用于所有系统 - 热库耦合参数范围的更通用的弛豫超算符。对一个模型二聚体的模拟再现了所有观测到的强耦合效应。