A discrete formulation of the theory of sojourn times in a two-state system

Most theoretical analyses of single-molecule spectroscopy (SMS) are formula ted in terms of a first-order isomerization process. The mathematical probl em to which the analysis reduces requires one to find the probability densi ty for the total residence time in one of the states at a given observation time T. In this paper we develop a slightly more rigorous theory in which account is taken of the discrete pulsing of the laser. It is shown how to p ass to the continuum limit. We develop analogous results to analyze experim ents in which the quantum yield is less than 1. (C) 2001 Published by Elsev ier Science B.V. All rights reserved.