以具有简单三能级结构染料分子的单量子系统为研究对象,用带有边界条件的速率方程来反映低功率单色连续激光激励下单分子发射荧光的动力学过程.该方法可以通过时间分辨光子探测获得处理单分子动力学随机过程.研究给出了一种通过求解反映单量子系统动力学过程的物理量——延迟函数计算关联函数的方法,并给出了双能级系统和双态系统延迟函数和关联函数的具体表达式.研究表明,在实际测量中只要获得关联函数曲线,就可以通过数据拟合计算出分子跃迁的动力学参量.
The three-level dye molecule single quantum system interacting with a cw laser field is investigated. The dynamic process of a single-molecule emitted photon is described by rate equations with absorbing boundary condition. It is demonstrated that the dynamics of the single-molecule processes and the statistics of time-resolved photon detection can be conveniently described in terms of renewal stochastic processes. The approach of calculating the correlation function by calculating the delay function that is an important physics quantity reflecting single quantum system dynamic process is given, and explicit expressions of correlation functions for two-levels and two-states systems are derived. This approach can be used for calculate dynamics parameter of molecular transition based on the fluorescence intensity correlation function.