Journal Article PUBDB-2023-07577

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High-harmonic spectroscopy of low-energy electron-scattering dynamics in liquids

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2023
Nature Publishing Group Basingstoke

Nature physics 19(12), 1813 - 1820 () [10.1038/s41567-023-02214-0]
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Abstract: High-harmonic spectroscopy is an all-optical nonlinear technique with inherent attosecond temporal resolution. It has been applied to a variety of systems in the gas phase and solid state. Here we extend its use to liquid samples. By studying high-harmonic generation over a broad range of wavelengths and intensities, we show that the cut-off energy is independent of the wavelength beyond a threshold intensity and that it is a characteristic property of the studied liquid. We explain these observations with a semi-classical model based on electron trajectories that are limited by the electron scattering. This is further confirmed by measurements performed with elliptically polarized light and with ab-initio time-dependent density functional theory calculations. Our results propose high-harmonic spectroscopy as an all-optical approach for determining the effective mean free paths of slow electrons in liquids. This regime is extremely difficult to access with other methodologies, but is critical for understanding radiation damage to living tissues. Our work also indicates the possibility of resolving subfemtosecond electron dynamics in liquids offering an all-optical approach to attosecond spectroscopy of chemical processes in their native liquid environment.

Classification:

Contributing Institute(s):
  1. Forschungsgruppe für strukturelle Dynamik (MPSD)
  2. MPSD (CFEL-MPT)
Research Program(s):
  1. 899 - ohne Topic (POF4-899) (POF4-899)
  2. DFG project G:(GEPRIS)194651731 - EXC 1074: Hamburger Zentrum für ultraschnelle Beobachtung (CUI): Struktur, Dynamik und Kontrolle von Materie auf atomarer Skala (194651731) (194651731)
  3. DFG project G:(GEPRIS)390715994 - EXC 2056: CUI: Advanced Imaging of Matter (390715994) (390715994)
Experiment(s):
  1. No specific instrument

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 Record created 2023-12-07, last modified 2025-07-24


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