Time-Dependent Fluctuations in Single Molecule Spectroscopy: A Generalized Wiener-Khintchine Approach

Abstract

We consider the theory of time-dependent fluctuations in single molecule spectroscopy. In particular, the relation between stationary spectral diffusion processes and photon counting statistics is investigated. Within linear response theory, a general relation between Mandel's Q parameter and a three time dipole correlation function is obtained. For a prototype spectral diffusion process, an exact solution of Q is found which exhibits rich types of physical behaviors.