Solvation-induced local structure in liquids probed by high-harmonic spectroscopy.

Area of Science:

• Quantum optics
• Physical chemistry
• Spectroscopy

Background:

• High-harmonic generation (HHG) is a key technique for probing quantum systems.
• Extending HHG spectroscopy to liquids is challenging but offers insights into solvation dynamics.
• Understanding HHG in liquids requires investigating the interplay between quantum systems and their local environment.

Purpose of the Study:

• Investigate high-harmonic generation in liquid binary solutions of aromatic benzene derivatives in methanol.
• Explore the potential of HHG spectroscopy as a nonlinear probe of solvation dynamics.
• Determine how localized solvation structures influence HHG spectra.

Main Methods:

• Experimental investigation of high-harmonic generation in liquid solutions.
• Systematic variation of laser parameters, concentration, and solute types (halogenated benzene derivatives).
• Theoretical interpretation guided by simulations of solvation effects.

Main Results:

• Observed suppression of specific harmonic orders and reduced total harmonic yield in HHG spectra.
• Evidence of a localized solvation structure acting as a scattering barrier.
• Characterization of solvation effects based on laser parameters and solution composition.

Conclusions:

• HHG spectroscopy in liquids can reveal detailed information about solvation structure and dynamics.
• Localized solvation shells significantly impact HHG spectra, acting as scattering barriers.
• This study expands the understanding of HHG mechanisms in condensed phases with short-range order.