Ultrafast transfer and transient entrapment of photoexcited Mg electron in Mg@C60

TL;DR

This study investigates ultrafast electron transfer in Mg@C60 endofullerene, revealing rapid charge transfer and transient electron trapping through advanced molecular dynamics simulations, with implications for experimental ultrafast spectroscopy.

Contribution

It demonstrates the ultrafast charge transfer and transient electron trapping in Mg@C60 using two complementary simulation methods, providing new insights into electron dynamics in endofullerenes.

Findings

Charge transfer occurs within tens of femtoseconds.

Transient electron trapping delays recombination.

Both simulation methods agree on ultrafast relaxation times.

Abstract

Electron relaxation is studied in endofullerene Mg@C60, after an initial localized photoexcitation in Mg, by nonadiabtic molecular dynamics simulations. To ensure reliability, two methods are used: i) an independent particle approach with a DFT description of the ground state and ii) HF ground state with many-body effects for the excited state dynamics. Both methods exhibit similar relaxation times leading to an ultrafast decay and charge transfer from Mg to C60 within tens of femtoseconds. Method (i) further elicits a robust transient-trap of the transferred electron that can delay the electron-hole recombination. Results shall motivate experiments to probe these ultrafast processes by two-photon transient absorption spectroscopy in gas phase, in solution, or as thin films.