Virtual Winter School on Computational Chemistry
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Institute of Physical and Theoretical Chemistry, Goethe University Frankfurt, Max von-Laue Str. 7, 60438 Frankfurt, Germany
Many elementary processes in functional organic materials involve ultrafast photoinduced energy and charge transfer, as highlighted by time-resolved spectroscopic observations. Coherent effects are found to play a major role, despite static and dynamic disorder. Hence, quantum dynamical methods are needed to elucidate the details of these ultrafast transfer events and capture the subtle interplay of site-to-site electronic couplings, exciton and charge delocalization, nonadiabatic effects and vibronic couplings. In this lecture, we review an approach that combines first-principles parametrized Hamiltonians , with accurate quantum dynamics simulations using the Multi-Layer Multi-Configuration Time-Dependent Hartree (MCTDH) method [1-4], along with semiclassical approaches [5,6]. The lecture will focus on (i) exciton dissociation and free carrier generation in regioregular donor-acceptor assemblies [1,7], and (ii) the elementary mechanism of exciton migration [5,6,8-10] and creation ofcharge-transfer excitons [7,11] in polythiophene and poly(para-phenylene vinylene) type materials. Special emphasis is placed on the interplay of trapping due to high-frequency phonon modes andthermal activation due to low-frequency ”soft” modes which drive a diffusive dynamics [6,9,10].
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