RhoDyn: A rho-TD-RASCI Framework to Study Ultrafast Electron Dynamics in Molecules

This article presents the program module RhoDyn as part of the OpenMOLCAS project intended to study ultrafast electron dynamics within the density-matrix-based time-dependent restricted active space configuration interaction framework (rho-TD-RASCI). The formalism allows for the treatment of spin-orbit coupling effects, accounts for nuclear vibrations in the form of a vibrational heat bath, and naturally incorporates (auto)ionization effects. Apart from describing the theory behind and the program workflow, the paper also contains examples of its application to the simulations of the linear L-2,L-3 absorption spectra of a titanium complex, high harmonic generation in the hydrogen molecule, ultrafast charge migration in benzene and iodoacetylene, and spin-flip dynamics in the core excited states of iron complexes.