Three-time correlation function, single molecule spectroscopy

In this chapter, we developed a stochastic theory of single molecule fluorescence spectroscopy. Fluctuations described by Q are evaluated in terms of a three-time correlation function C iXi, X2, T3) related to the response function in nonlinear spectroscopy. This function depends on the characteristics of the spectral diffusion process. Important time-ordering properties of the three-time correlation function were investigated here in detail. Since the fluctuations (i.e., Q) depend on the three-time correlation function, necessarily they contain more information than the line shape that depends on the one-time correlation function Ci(ti) via the Wiener-Khintchine theorem. 

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