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

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.

8 pages, 7 figures

References in corpus (5)

• NWChem: Past, Present, and Future
• Libxc: a library of exchange and correlation functionals for density functional theory
• Attosecond Coherent Electron Motion in Auger-Meitner Decay
• Control of charge migration in molecules by ultrashort laser pulses
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Cited by in corpus (4)

• All-Electron, Density Functional-Based Method for Angle-Resolved Tunneling Ionization in the Adiabatic Regime
• Tracking Charge Migration with Frequency-Matched Strobo-Spectroscopy
• Simulating real-time molecular electron dynamics efficiently using the time-dependent density matrix renormalization group
• High Harmonic Generation from Isolated Bound States: Tunable Emission Spectra and Mollow Triplets