Modeling charge transport in high-mobility molecular semiconductors: Balancing electronic structure and quantum dynamics methods with the help of experiments.

Computing the charge mobility of molecular semiconductors requires a balanced set of approximations covering both the electronic structure of the Hamiltonian parameters and the modeling of the charge dynamics. For problems of such complexity, it is hard to make progress without independently validating each layer of approximation. In this perspective, we survey how all terms of the model Hamiltonian can be computed and validated by independent experiments and discuss whether some common approximations made to build the model Hamiltonian are valid. We then consider the range of quantum dynamics approaches used to model the charge carrier dynamics stressing the strong and weak points of each method on the basis of the available computational results. Finally, we discuss non-trivial aspects and novel opportunities related to the comparison of theoretical predictions with recent experimental data.