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Quantum dynamics of ultrafast photoinduced processes in organic semiconductors: exciton dissociation at polymer heterojunctions

A molecular‐level, quantum‐dynamical analysis of phonon‐driven exciton dissociation in semiconducting polymers is presented, using a linear vibronic coupling model in conjunction with a recently developed hierarchical chain representation. Quantum‐dynamical simulations in 20‐30 dimensions are carried out using efficient multiconfigurational techniques. The decay of the exciton towards a charge‐separated state is shown to be an ultrafast, coherent process of pronounced non‐equilibrium character, which cannot be modeled by conventional kinetic equations. (© 2008 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)