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Donor-acceptor molecules with 4-(dimethylamino)phenyl donor and 1,1,4,4-tetracyanobuta-1,3-diene acceptor moieties are readily prepared by short, high-yielding routes. The quite small chromophores are characterised by X-ray crystallography and feature intense intramolecular charge-transfer bands, substantial quinoid character in the donor rings, reversible electrochemical reductions and oxidations and powerful third-order optical nonlinearities.

We visualize exciton diffusion in rubrene single crystals using localized photoexcitation and spatially resolved detection of excitonic luminescence. We show that the exciton mobility in this material is strongly anisotropic with long-range diffusion by several micrometers associated only with the direction of molecular stacking in the crystal, along the b axis. We determine a triplet exciton diffusion length of 4.0 ± 0.4 μm from the spatial exponential decay of the photoluminescence that originates from singlet excitons formed by triplet-triplet fusion.

The decay of the photoluminescence excited in rubrene single crystals by picosecond pulses is measured over 7 orders of magnitude and more than 4 time decades. We identify the typical decay dynamics due to triplet-triplet interaction. We show that singlet exciton fission and triplet fusion quantum yields in rubrene are both very large, and we directly determine a triplet exciton lifetime of 100 ± 20 μs, which explains the delayed buildup of a large photocurrent that has been reported earlier for low excitation densities.