Speaker: Frank Ortmann, Technical University of Munich

Understanding charge and exciton dynamics in molecular systems is critical for advancing organic semiconductor and optoelectronic technologies. We present insights from our work addressing distinct yet complementary aspects of these phenomena for organic electronic materials. First, we explore charge-transfer dynamics in electron-phonon coupled model systems, identifying regimes such as transient localization and polaron transport, emphasizing their seamless transitions across vibrational modes and temperatures. Second, a comparative analysis of the Matrix Product State (MPS) and Multilayer Multiconfiguration Time-Dependent Hartree (MCTDH) methods demonstrates their efficacy in modeling non-adiabatic exciton dissociation, revealing specific sensitivities to electronic-vibrational entanglement in complex systems. Finally, a quantum mechanical assessment of ultrafast charge transfer at donor-acceptor interfaces benchmarks MPS against semi-classical hopping models, showcasing their convergence while highlighting the role of vibrational dynamics in optimizing photovoltaic performance. These works underline the importance of methodical and theoretical advances in capturing the interplay of electronic and vibrational degrees of freedom in molecular optoelectronics.