Ultrafast excitonic and charge transfer dynamics in nanostructured organic polymer materials

We present theoretical studies of elementary exciton and charge transfer processes in functional organic materials, in view of understanding the key microscopic factors that lead to efficient charge generation in photovoltaics applications. As highlighted by recent experiments, these processes can be guided by quantum coherence, despite the presence of static and dynamic disorder. Our approach combines first-principles parametrized Hamiltonians, based on Time-Dependent Density Functional Theory (TDDFT) and/or high-level electronic structure calculations, with accurate quantum dynamics simulations using the Multi-Configuration Time-Dependent Hartree (MCTDH) method. This contribution specifically addresses charge generation in a novel class of highly ordered oligothiophene-perylene diimide type co-oligomer assemblies, highlighting that chemical design of donor/acceptor combinations needs to be combined with a detailed understanding of the effects of molecular packing.