Modeling Charge Transfer in Fullerene Collisions via Real-Time Electron Dynamics

Jacek Jakowski; Stephan Irle; Bobby G Sumpter; Keiji Morokuma

doi:10.1021/jz3004377

Modeling Charge Transfer in Fullerene Collisions via Real-Time Electron Dynamics

J Phys Chem Lett. 2012 Jun 7;3(11):1536-42. doi: 10.1021/jz3004377. Epub 2012 May 23.

Authors

Jacek Jakowski¹, Stephan Irle², Bobby G Sumpter, Keiji Morokuma^{3

4}

Affiliations

¹ †National Institute for Computational Sciences, Oak Ridge, Tennessee 37831, United States.
² ‡Department of Chemistry, Graduate School of Science, Nagoya University, Nagoya 464-8602, Japan.
³ §Cherry Emerson Center for Scientific Computing and Department of Chemistry, Emory University, 1515 Dickey Drive, Atlanta, Georgia 30322, United States.
⁴ ∥Fukui Institute for Fundamental Chemistry, Kyoto University, Sakyo, Kyoto 6006-8103, Japan.

PMID: 26285634
DOI: 10.1021/jz3004377

Abstract

An approach for performing real-time dynamics of electron transfer in a prototype redox reaction that occurs in reactive collisions between neutral and ionic fullerenes is discussed. The quantum dynamical simulations show that the electron transfer occurs within 60 fs directly preceding the collision of the fullerenes, followed by structural changes and relaxation of electron charge. The consequences of real-time electron dynamics are fully elucidated for the far from equilibrium processes of collisions between neutral and multiply charged fullerenes.

Keywords: DFTB; Liouville−von Neumann molecular dynamics (LvNMD); TD-DFTB; carbon materials; electron friction; energy transfer; nonadiabatic coupling; nonequilibrium processes; quantum dynamics; redox reactions; time-dependent phenomena.