a comparison among DFT models*

Studies of the relaxation dynamics of photoexcited electrons in fullerene materials have applications in organic photovoltaics and medical photothermal therapy. In this work, we use an approach of electron-phonon coupled nonadiabatic molecular dynamics [1], based on density functional theory (DFT) [2-3], to simulate such relaxation process in C₆₀. The methodology relies on a combination of the fewest-switch surface hopping approach and Kohn−Sham single-particle description [2]. We calculate the femtosecond evolution of the population of initial excited states and of various intermediate states. A comparison of results obtained using the PBE, PBE0, and B3LYP exchange-correlation functional, will be presented. The population lifetimes are found to reflect the structure of unoccupied band which may inspire experiments in laser two-photon schemes.  [1] M. Madjet et al., Phys. Rev. Lett. 126, 183002, (2021); [2] A V. Akimov and O.V Prezhdo, J. Chem. Theory Comput. 9, 11 (2013); [3] M. Madjet et al. J. Phys. Chem. Lett 8, 18 (2017).