Light-induced nonadiabatic energy- and charge transfer dynamics

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The aim of the present project is the development of an efficient mixed quantum-classical methodology for the simulation of light-induced nonadiabatic dynamical processes in multichromophoric molecular aggregates. The dynamics of energy and charge transfer in such systems represents a hot topic of the state-of-the-art experimental research The energy and charge transfer dynamics in these systems is a hot topic of the state-of-the-art experimental research and there is growing evidence that nonadiabatic radiationless relaxation processes play a fundamental role in determining the efficiency of the exciton transfer or charge transport. In addition to the intramolecular nonradiative transitions through conical intersections, which play a fundamental role in photochemistry and photophysics, the coupling between the individual chromophores in multichromophoric assemblies gives rise to novel intermolecular nonradiative relaxation channels through funnels between the delocalized excitonic and/or charge transfer states. To simulate the energy and charge transfer dynamics in multichromophoric nanostructures we will develop and implement a combined methodology of light-induced surface hopping methods and efficient electronic structure calculations based on the long-range corrected time-dependent density functional tight-binding method. In order to directly compare our theoretical results with experimental findings and to support the interpretation of the latter, we will supplement our method by developing a theoretical approach for the simulation of time-resolved multidimensional spectra. This methodology will be applied for the simulation of the conformational dynamics and light-induced dynamical processes of squaraine oligomers in different solvent environments.