Journal Articles The Journal of Chemical Physics Year : 2025

Polarization Resolved Second Harmonic Scattering of Neat Water in the Right Angle and Forward Scattering Geometries

Abstract

Liquid water still remains an ubiquitous liquid the molecular organization of which requires careful investigation. In this work, we present a study of the second harmonic scattering (SHS) intensity for two different scattering angles, namely the forward and the right angle geometries.This method performed at optical wavelengths is indeed selective towards long correlation lengths. A polarization analysis demonstrates that it is then possible to clearly evidence a coherent component to the total SHS intensity using a fast Fourier transform analysis of the SHS intensity as a function of the fundamental angle of polarization despite its weak relative contribution.A model is then derived based on the rotational invariants to fully unravel the different contributions to the SHS intensity for the two right angle and forward angles of scattering as well as the dependence with the fundamental beam polarization angle. This model fully supports the experimental results further confirming an azimuthal geometry of the water-water orientational correlation function in neat water.
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Year Month Jours
Avant la publication
Tuesday, July 15, 2025
Embargoed file
Tuesday, July 15, 2025
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Dates and versions

hal-04888327 , version 1 (15-01-2025)

Identifiers

Cite

Fabien Rondepierre, Estelle Salmon, Christian Jonin, Julien Duboisset, Pierre-Francois Brevet. Polarization Resolved Second Harmonic Scattering of Neat Water in the Right Angle and Forward Scattering Geometries. The Journal of Chemical Physics, 2025, 162, pp.034201. ⟨10.1063/5.0243331⟩. ⟨hal-04888327⟩
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