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