Laser-Induced Circular Charge Migration in Endohedral Fullerenes in the Presence of Ionization

In this study, we explore the behavior of endohedral fullerenes and examine how different doping species influence the ultrafast photoinduced electronic dynamics. We analyzed a reference fullerene (C₆₀) and two endohedral fullerenes with Cl^– and Mg atoms inside the cage using electronic dynamics calculations. By applying circularly polarized light, we observed the transfer of angular momentum from the light to the electron density in these systems. The optical properties and specific excitations were determined through quantum chemical calculations, which formed the basis of our analysis. In the C₆₀ reference system, excitation led to a significant rotation of the electron density and the formation of a large rotating dipole. For the Mg@C60 system, the electron density changes were mostly localized around the Mg atom, resulting in a smaller induced dipole but more localized excitations. In the Cl^–@C₆₀ system, minimal angular momentum transfer was observed with an isotropic distribution of charges due to the charge-transfer nature of the excitations. The distinct behaviors observed in these systems highlight the diverse phenomena that can arise and represent a significant step toward developing novel molecular devices.