Ultrafast Quantum Dynamics of Functional Organic Polymer Materials : Coherence, Confinement, and Disorder

Orateur : Irene BURGHARDT

This talk addresses quantum dynamical studies of ultrafast photo-induced energy and charge transfer in functional organic materials, complementing time-resolved spectroscopic observations that underscore the coherent nature of the ultrafast elementary transfer events in these molecular aggregate systems [1]. The intricate interplay of electronic delocalization, coherent vibronic dynamics, and trapping phenomena requires a quantum dynamical treatment that goes beyond conventional mixed quantum-classical simulations. Our approach combines first-principles parametrized Hamiltonians [2], with accurate quantum dynamics simulations using the Multi-Configuration Time-Dependent Hartree (MCTDH) method [3] and its multi-layer (ML-MCTDH) variant [4], along with semiclassical approaches [5]. This talk will specifically focus on (i) exciton dissociation and free carrier generation in regioregular donor-acceptor assemblies [2,6], and (ii) the elementary mechanism of exciton migration [5,7,8] and creation of charge-transfer excitons [9] in polythiophene type donor materials. Special emphasis is placed on the influence of structural and dynamic disorder and molecular packing, which can act as a determining factor in transfer e-ciencies. Against this background, we will comment on the role of temporal and spatial coherence along with a consistent description of the transition to a classical-statistical regime.

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