Open quantum system simulation of time and frequency resolved spectroscopy

TL;DR

This paper presents a simulation approach for modeling the dynamics of excitonic energy transfer in molecular complexes using open quantum systems, linking physical processes to spectroscopic measurements.

Contribution

It introduces a method for simulating time and frequency resolved spectroscopy of open quantum systems in molecular complexes.

Findings

Effective modeling of energy transfer dynamics

Connection between decoherence, relaxation, and spectroscopy

Insights into vibrational mode effects

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.