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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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
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ATOMIC AND MOLECULAR PHYSICS
Chemical physics & physical chemistry
High-order harmonic generation
Optics
Physics
Time-dependent DFT
Ultrafast phenomena
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cited_by cdi_FETCH-LOGICAL-c321t-6c14c39894c86566c1f8866ea6ffc390848706ad5c6145cc6745cc9505197a293
cites cdi_FETCH-LOGICAL-c321t-6c14c39894c86566c1f8866ea6ffc390848706ad5c6145cc6745cc9505197a293
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container_issue 1
container_start_page
container_title Physical review. A
container_volume 106
creator Hamer, Kyle A.
Mauger, François
Folorunso, Aderonke S.
Lopata, Kenneth
Jones, Robert R.
DiMauro, Louis F.
Schafer, Kenneth J.
Gaarde, Mette B.
description 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.
doi_str_mv 10.1103/PhysRevA.106.013103
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source American Physical Society:Jisc Collections:APS Read and Publish 2023-2025 (reading list)
subjects ATOMIC AND MOLECULAR PHYSICS
Chemical physics & physical chemistry
High-order harmonic generation
Optics
Physics
Time-dependent DFT
Ultrafast phenomena
title Characterizing particle-like charge-migration dynamics with high-order harmonic sideband spectroscopy
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