Reichman David R
Department of Chemistry, Columbia University, 3000 Broadway, New York, New York, 10025, USA.
J Phys Chem B. 2006 Sep 28;110(38):19061-5. doi: 10.1021/jp061992j.
In this paper we investigate some general aspects of stochastic models of dynamic disorder. First, we reexamine the Zwanzig model for the kinetics of escape through a fluctuating hole. We show that this model is trivially connected to the canonical model of the broadening of the zero-phonon line (ZPL) in crystals. This provides a new perspective of the Wang-Wolynes expression for the rate of escape from a geometric bottleneck with non-Markovian Gaussian fluctuations. Motivated by recent single-molecule experiments, we examine more general examples of fluctuation processes from the perspective of cumulant expansions. Finally, we discuss recent single-molecule experiments probing enzyme turnover performed by Xie and co-workers.
在本文中,我们研究了动态无序随机模型的一些一般方面。首先,我们重新审视了通过波动孔逃逸动力学的兹万齐格模型。我们表明,该模型与晶体中零声子线(ZPL)展宽的规范模型存在简单联系。这为从具有非马尔可夫高斯涨落的几何瓶颈逃逸速率的王 - 沃利内斯表达式提供了新视角。受近期单分子实验的启发,我们从累积量展开的角度研究了更一般的涨落过程示例。最后,我们讨论了谢及其同事进行的探测酶周转的近期单分子实验。