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We present a comparative study of ultrafast photo-conversion dynamics intetracene (Tc) and pentacene (Pc) single crystals and Pc films using opticalpump-probe spectroscopy. Photo-induced absorption in Tc and Pc crystals isactivated and temperature-independent respectively, demonstrating dominantsinglet-triplet exciton fission. In Pc films (as well as C$_{60}$-doped films)this decay channel is suppressed by electron trapping. These resultsdemonstrate the central role of crystallinity and purity in photogenerationprocesses and will constrain the design of future photovoltaic devices.

Morphology Effectively Controls Singlet-Triplet Exciton Relaxation and Charge Transport in Organic Semiconductors