Title: Molecular Modes of Attosecond Charge Migration

Aderonke S. Folorunso [1], Adam Bruner [1], François Mauger [2], Kyle A. Hamer [2], Samuel Hernandez [1], Robert R. Jones [3], Louis F. DiMauro [4], Mette B. Gaarde [2], Kenneth J. Schafer [2], and Kenneth Lopata [1,5]

[1] Department of Chemistry, Louisiana State University, Baton Rouge, Louisiana 70803, USA

[2] Department of Physics and Astronomy, Louisiana State University, Baton Rouge, Louisiana 70803, USA

[3] Department of Physics, University of Virginia, Charlottesville, Virginia 22904, USA

[4] Department of Physics, The Ohio State University, Columbus, Ohio 43210, USA

[5] Center for Computation and Technology, Louisiana State University, Baton Rouge, Louisiana 70808, US

Abstract:

First-principles calculations are employed to elucidate the modes of attosecond charge migration (CM) in halogenated hydrocarbon chains. We use constrained density functional theory (DFT) to emulate the creation of a localized hole on the halogen, and follow the subsequent dynamics via time-dependent DFT. We find low-frequency CM modes (~1 eV) that propagate across the molecule and study their dependence on length, bond order, and halogenation. We observe that the CM speed is largely independent of molecule length, but is lower for triple-bonded versus double-bonded molecules. Additionally, as the halogen mass increases the hole travels in a more particle-like manner as it moves across the molecule. These heuristics will likely prove useful in identifying molecules and optimal CM detection methods for future experiments, especially for halogenated hydrocarbons which are promising targets for ionization-triggered CM.

Status: Published, Phys. Rev. Lett. 126, 133002 (2021).