Studies of vibrational relaxation of photoexcited electrons in endofullerene molecules

Using a density functional theory-based scheme of non-adiabatic molecular dynamics simulations [1,2], the electron relaxation dynamics in a prototypical endofullerene Mg@C₆₀ after an initial localized photoexcitation in Mg is investigated. Two approaches to the electronic structure of the excited electronic states are used [3]: (i) an independent particle approximation based on a density functional theory description of molecular orbitals and (ii) a configuration-interaction description of the many-body effects. Results of electronic properties, optical excitations and ultrafast population decay dynamics will be presented. The effect of different exchange-correlation (XC) functionals will be discussed. The advantages and drawbacks of the two methods will be outlined.

 [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., (Submitted) http://arxiv.org/abs/2012.00705