We present a model of charge transport in organic molecular semiconductors based on the effects of lattice fluctuations on the quantum coherence of the electronic state of the charge carrier. Thermal intermolecular phonons and librations tend to localize pure coherent states and to assist the motion of less coherent ones. Decoherence is thus the primary mechanism by which conduction occurs. It is driven by the coupling of the carrier to the molecular lattice through polarization and transfer integral fluctuations as described by the Hamiltonian of Gosar and Choi [Phys. Rev. 150, 529 (1966)]. Localization effects in the quantum coherent regime are modeled via the Anderson Hamiltonian with correlated diagonal and nondiagonal disorders [M.-N. Bussac et al., Europhys. Lett. 66, 392 (2004)] leading to the determination of the carrier localization length. This length defines the coherent extension of the ground state and determines, in turn, the diffusion range in the incoherent regime and thus the mobility. The transfer integral disorder of Troisi and Orlandi [J. Phys. Chem. A 110, 4065 (2006)] can also be incorporated. This model, based on the idea of decoherence, allowed us to predict the value and temperature dependence of the carrier mobility in prototypical organic semiconductors that are in qualitative accord with experiments.

• Received 19 September 2006

DOI:https://doi.org/10.1103/PhysRevB.75.235106