Probing single molecule kinetics by photon arrival trajectories

Multitime correlation functions of photon arrival times in single molecule fluorescence resonant energy transfer measurements are computed using a simple model representing slow conformational dynamics described by a collective stochastic Gaussian coordinate. The analogy with time domain nonlinear optical spectroscopy is explored. Various statistical measures of distributions of single photon arrival times and fluorescence lifetimes are employed to analyze non-Poissonian statistics. (C) 2002 American Institute of Physics.