Cao Jianshu
Department of Chemistry, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA.
J Phys Chem B. 2006 Sep 28;110(38):19040-3. doi: 10.1021/jp061302b.
Multiple time scales are the intrinsic nature of complex systems and can be revealed through single molecule photon statistical analysis. The standard Poisson indicator defined by the time-averaged initial condition measures photon bunching and antibunching but cannot be directly related to multiple time scales. A new indicator defined by the event-averaged initial condition is proposed to detect the deviation from the renewal behavior and to directly probe the effects of conformational fluctuations. Detailed calculations of modulated two-level systems are carried out using the transfer matrix method to demonstrate the difference between the two indicators. The relationship between ensemble-averaged survival probabilities and photon statistics is also explored in the context of single molecule measurements.
多时间尺度是复杂系统的固有特性,可通过单分子光子统计分析揭示。由时间平均初始条件定义的标准泊松指标测量光子聚束和反聚束,但不能直接与多时间尺度相关联。提出了一种由事件平均初始条件定义的新指标,以检测与更新行为的偏差并直接探测构象波动的影响。使用转移矩阵方法对调制二能级系统进行了详细计算,以证明这两个指标之间的差异。在单分子测量的背景下,还探讨了系综平均生存概率与光子统计之间的关系。