Modeling of Transient Absorption Spectra in Exciton–Charge-Transfer Systems

• DOI: 10.1021/acs.jpcb.6b09858
• Publication Date: 2016-12-21T19:17:29Z
• Authors: Tobias Kramer; Mirta Rodríguez; Yaroslav Zelinskyy
• Keywords: Chemical Physics (physics.chem-ph); Time Factors; Light; Spectrum Analysis; Light-Harvesting Protein Complexes; Temperature; FOS: Physical sciences; Molecular Dynamics Simulation; 01 natural sciences; 7. Clean energy; 0104 chemical sciences; Energy Transfer; Physics - Chemical Physics

Time-resolved spectroscopy provides the main tool for analyzing the dynamics of excitonic energy transfer in light-harvesting complexes. To infer time-scales and effective coupling parameters from experimental data requires to develop numerical exact theoretical models. The finite duration of the laser-molecule interactions and the reorganization process during the exciton migration affect the location and strength of spectroscopic signals. We show that the non-perturbative hierarchical equations of motion (HEOM) method captures these processes in a model exciton system, including the charge transfer state.