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The great majority of electronic and optoelectronic devices depends oninterfaces between n-type and p-type semiconductors. Finding such matchingdonor-acceptor systems in molecular crystals remains a challenging endeavor.Structurally compatible molecules may not necessarily be suitable with respectto their optical and electronic properties: large exciton binding energies mayfavor bound electron-hole pairs rather than charge separation by excitondissociation, and free, band-like transport is challenging to achieve ashopping commonly dominates charge motion. Structurally well-definedpentacene-perfluoropentacene heterostructures in different polymorphs andmolecular orientations are model systems to study the relation of packing motifand optical properties. These heterosystems feature two characteristicinterface-specific luminescence channels at around 1.4 and 1.5 eV. Theirrelative emission strength strongly depends on the molecular alignment of therespective donor and acceptor molecules. Evaluating their dynamics incomparison with the corresponding unitary films reveals the role ofsinglet-triplet intersystem crossing and different channels for carrierinjection into the interface-specific resonances.

Molecular Packing Motifs Determine Charge-Transfer and Carrier Dynamics in Molecular Heterosystems: the Case of Pentacene - Perfluoropentacene