Title: Characterizing Particle-Like Charge Migration Dynamics with High-Harmonic Sideband Spectroscopy

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

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

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

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

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

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

Abstract:

We introduce high-harmonic sideband spectroscopy (HHSS) and show that it can be a robust probe of attosecond charge migration (CM) in a halogenated carbon-chain molecule. We simulate both the CM and harmonic-generation (HHG) dynamics using ab initio time-dependent density-functional theory. We find that CM dynamics initiated along the molecular backbone induces sidebands in the HHG spectrum driven by a delayed laser pulse that is polarized perpendicular to the molecular axis. Monitoring the spectrum as either the HHG laser frequency or the relative delay is scanned allows for the extraction of detailed information about the time-domain characteristics of the CM process.

Status: Published, Phys. Rev. A 106, 013103 (2022).