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

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...

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Bibliographic Details
Published in:arXiv.org 2022-05
Main Authors: Hamer, Kyle A, Mauger, Francois, Folorunso, Aderonke S, Lopata, Kenneth, Jones, Robert R, DiMauro, Louis F, Schafer, Kenneth J, Gaarde, Mette B
Format: Article
Language:English
Subjects:
Density functional theory
Molecular chains
Sidebands
Spectroscopy
Spectrum analysis
Time dependence
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Summary: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.
ISSN:2331-8422
DOI:10.48550/arxiv.2202.00730