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


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Date

2023-12

Publication Type

Journal Article

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yes

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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.

Publication status

published

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Volume

19 (12)

Pages / Article No.

1813 - 1820

Publisher

Nature

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Organisational unit

03888 - Wörner, Hans Jakob / Wörner, Hans Jakob check_circle

Notes

Funding

172946 - Soft-X-ray spectroscopy on the attosecond time scale (SNF)
204928 - Attosecond chemistry in the gas and liquid phases (SNF)

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