Ultrafast Transfer and Transient Entrapment of Photoexcited Mg Electron in Mg@C_{60}.

Phys Rev Lett

Department of Natural Sciences, D. L. Hubbard Center for Innovation, Northwest Missouri State University, Maryville, Missouri 64468, USA.

Published: May 2021

Electron relaxation is studied in endofullerene Mg@C_{60} after an initial localized photoexcitation in Mg by nonadiabatic molecular dynamics simulations. Two approaches to the electronic structure of the excited electronic states are used: (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. Both methods exhibit similar relaxation times, leading to an ultrafast decay and charge transfer from Mg to C_{60} within tens of femtoseconds. Method (i) further elicits a 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 or photoelectron spectroscopy in gas phase, in solution, or as thin films.

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http://dx.doi.org/10.1103/PhysRevLett.126.183002DOI Listing

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