Understanding the encapsulation and release processes of drug molecules using nanocarriers is vital for the development of nanoscale drug delivery.

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The trajectory surface hopping (TSH) method is nowadays widely applied to study the charge/exciton transport process in organic semiconductors (OSCs). In the present study, we systematically examine the performance of two approximations in the fewest switched surface hopping (FSSH) simulations for charge transport (CT) in several representative OSCs. These approximations include (i) the substitution of the nuclear velocity scaling along the nonadiabatic coupling vector (NCV) by rescaling the hopping probability with the Boltzmann factor (Boltzmann correction (BC)) and (ii) a phenomenological approach to treat the quantum feedback from the electronic system to the nuclear system (implicit charge relaxation (IR)) in the OSCs. We find that charge mobilities computed by FSSH-BC-IR are in very good agreement with the mobilities obtained by standard FSSH simulations with explicit charge relaxation (FSSH-ER), however, at reduced computational cost. A key parameter determining the charge carrier mobility is the reorganization energy, which is sensitively dependent on DFT functionals applied. By employing the IR approximation, the FSSH method allows systematic investigation of the effect of the reorganization energies obtained by different DFT functionals like B3LYP or ωB97XD on CT in OSCs. In comparison to the experiments, FSSH-BC-IR using ωB97XD reorganization energy underestimates mobilities in the low-coupling regime, which may indicate the lack of nuclear quantum effects (e.g., zero point energy (ZPE)) in the simulations. The mobilities obtained by FSSH-BC-IR using the B3LYP reorganization energy agree well with experimental values in 3 orders of magnitude. The accidental agreement may be the consequence of the underestimation of the reorganization energy by the B3LYP functional, which compensates for the neglect of nuclear ZPE in the simulations.

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