Ultrafast hot-carrier relaxation in photoexcited Ca@C₆₀ molecule

We investigate the processes of hot-carrier relaxation in photoexcited Ca@C₆₀ molecule at room temperature by using a scheme based on ab initio nonadiabatic molecular dynamics simulations and time-dependent density functional theory [1-3]. The methodology is underpinned by a combination of the fewest-switch surface hopping approach and Kohn−Sham single-particle description. Results indicate that the relaxation of the excited population to the band edges occurs on the ultrafast time scale driven by the dynamical electron-phonon coupling. We will investigate the population lifetimes for unoccupied orbital states near the energy gap and study the role of spin multiplicity in the hot-carrier relaxation process in Ca@C₆₀. Some results will be presented in the conference.

[1] A. V. Akimov and O.V Prezhdo, J. Chem. Theory Comput. 9, 11 (2013); [2] Madjet et al., J. Phys. Chem. Lett. 8, 18 (2017) ;[3] Madjet et al., Phys. Rev. Lett. 126, 183002 (2021)