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We present comprehensive study of ultrafast charge carrier dynamics in a variety of organic molecular crystals. In all samples, we observed sub-picosecond charge photogeneration and band-like transport, characterized by (i) an increase in charge carrier mobility as the temperature decreases in a wide temperature range of at least 20 K – 300 K and (ii) mobility anisotropy in the a-b plane of the crystals. The temperature dependence of the decay dynamics of the transient photoconductivity reveals the presence of shallow trapping sites in herring-bone-type-structured crystals (such as pentacene (Pc), tetracene (Tc), and rubrene (Rub)), while such traps are apparently absent in “brick-wall”-type crystals (such as functionalized pentacene (FPc)). We also report on the measurements of the charge carrier mobility anisotropy in the a-b plane of two types of FPc single crystals. Anisotropies of approximately 3.5 and 11.6 were obtained in the crystals characterized by crystal structures favoring two-dimensional and one-dimensional charge transport, respectively, consistent with the degree of π-overlap along different directions in the crystals.
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