Unveiling unique ultrafast nonlinearities in liquid-phase high-order harmonic generation

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Abstract
High-order harmonic generation (HHG) provides a powerful optical tool for probing ultrafast dynamics on the attosecond timescale. While its mechanisms in gases and solids are well-established, understanding nonlinear optical responses in liquids remains challenging. The absence of long-range order in liquids questions the applicability of the existing HHG models developed in other media. Through combined experimental and theoretical investigations, we identify unique characters of liquid-phase HHG-spectral redshift and broadening, which are fundamentally distinct from both the gaseous and solid-state counterparts. Quantitative measurements and simulations of HHG in liquids illustrate a near linear dependence of harmonic redshift and broadening on the laser intensity, with the nonlinear response of water exceeding that of ethanol. The simulations reveal that these features arise from delocalized electronic states with energy loss in multiple scatterings and transient Stark shift during their transitions in laser fields. Meanwhile, we find that liquid polarity or hydrogen bond exerts decisive control over the transition dipole momentum distributions of delocalized states. Our findings establish a nonlinear spectral method for probing the internal network in liquids, paving the way for studying its role in chemical and biological processes.

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