Generating function methods in single-molecule spectroscopy.

Certain single-molecule measurements record a time series of individual physical events. Examples of such events include the emission of single photons or discrete fluctuations of molecular state (as in fluorescence blinking or spectral diffusion). The generating function formalism is a natural framework for studying these measurements both theoretically and numerically. Kinetic, stochastic, and quantum models for chromophore dynamics may all be extended to generating function calculations, enabling direct comparison to experiment with only slight extensions to familiar theoretical/computational tools.