Open quantum system simulation of time and frequency resolved spectroscopy

Abstract

The dynamics of excitonic energy transfer in molecular complexes triggered by interaction with laser pulses offers a unique window into the underlying physical processes. The absorbed energy moves through the network of interlinked pigments and in photosynthetic complexes reaches a reaction center. The efficiency and time-scale depend not only on the excitonic couplings, but are also affected by the dissipation of energy to vibrational modes of the molecules. An open quantum system description provides a suitable tool to describe the involved processes and connects the decoherence and relaxation dynamics to measurements of the time-dependent polarization.