Abstract
Second harmonic scattering (SHS) is a method of choice to investigate the molecular structure of liquids. While a clear interpretation of SHS intensity exists for diluted solutions of dyes, the scattering due to solvents remains difficult to interpret quantitatively. Here, we report a quantum mechanics/molecular mechanics (QM/MM) approach to model the polarization-resolved SHS intensity of liquid water, quantifying different contributions to the signal. We point out that the molecular hyperpolarizability fluctuations and correlations cannot be neglected. The intermolecular orientational and hyperpolarizability correlations up to the third solvation layer strongly increase the scattering intensities and modulate the polarization-resolved oscillation that is predicted here by QM/MM without fitting parameters. Our approach can be generalized to other pure liquids to provide a quantitative interpretation of SHS intensities in terms of short-range molecular ordering.
Talk to us
Join us for a 30 min session where you can share your feedback and ask us any queries you have
Schedule a callDisclaimer: All third-party content on this website/platform is and will remain the property of their respective owners and is provided on "as is" basis without any warranties, express or implied. Use of third-party content does not indicate any affiliation, sponsorship with or endorsement by them. Any references to third-party content is to identify the corresponding services and shall be considered fair use under The CopyrightLaw.
