Principles of modeling the fluorescence spectral dynamics of dye molecules in solutions

FSDS is Fluorescence Spectral Dynamics Simulator, designed to investigate photoinduced charge transfer and its manifestations in time-resolved fluorescence spectra of a dye in a solvent. The project is implemented in C, using the MPI library. The computer model simulates stationary absorption and fluorescence spectra, as well as the time evolution of population distributions along the solvent reaction coordinate, to calculate spectral dynamics. Excitation and relaxation of intramolecular high-frequency vibrations are described at the quantum level. FSDS can fit the physical parameters of the dyes to experimental data. The dye excitation is consistently described accounting for the finite duration of the pump pulse. The program code implements two evolutionary models: a spin-boson model within the harmonic potential and a stochastic model based on the Smoluchowski diffusion operator for an arbitrary free energy surface. Computer simulation shows the numerical coincidence of the calculations performed in the framework of these models for the harmonic free energy surface. The detail description of the code and numerical schemes are presented.