Characterizing particle-like charge-migration dynamics with high-order harmonic sideband spectroscopy

Here, we introduce high-order harmonic sideband spectroscopy and show that it can be a robust probe of charge migration (CM) in a halogenated carbon-chain molecule. We simulate both the CM and high-order harmonic generation (HHG) dynamics using ab initio time-dependent density-functional theory. We...

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Bibliographic Details
Published in:Physical review. A 2022-07, Vol.106 (1), Article 013103
Main Authors: Hamer, Kyle A., Mauger, François, Folorunso, Aderonke S., Lopata, Kenneth, Jones, Robert R., DiMauro, Louis F., Schafer, Kenneth J., Gaarde, Mette B.
Format: Article
Language:English
Subjects:
ATOMIC AND MOLECULAR PHYSICS
Chemical physics & physical chemistry
High-order harmonic generation
Optics
Physics
Time-dependent DFT
Ultrafast phenomena
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Summary:Here, we introduce high-order harmonic sideband spectroscopy and show that it can be a robust probe of charge migration (CM) in a halogenated carbon-chain molecule. We simulate both the CM and high-order 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:2469-9926
2469-9934
DOI:10.1103/PhysRevA.106.013103