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Updated: Jul 16, 2026

Probing the Structure and Dynamics of Interfacial Water with Scanning Tunneling Microscopy and Spectroscopy
Published on: May 27, 2018
Comment on "Water-water correlations in electrolyte solutions probed by hyper-Rayleigh scattering" [J. Chem. Phys.
Y Chen1, H I Okur1, N Dupertuis1
1Laboratory for Fundamental BioPhotonics (LBP), Institutes of Bio-Engineering (IBI) and Materials Science (IMX) and Lausanne Center for Ultrafast Science (LACUS), Lausanne, Switzerland.
Abstract:
The work by Shelton [J. Chem. Phys. 147, 214505 (2017)] discussed and interpreted differences with a previous study by Chen et al. [Sci. Adv. 2, e1501891 (2016)] regarding the influence of electrolytes on the structure of water. It is argued by Shelton [J. Chem. Phys. 147, 214505 (2017)] that impurities and hyper-Raman scattering contributions are the reasons for differences in the measured second harmonic intensity between the above two studies. Here, we show that these proposed effects are not relevant and discuss the influence of pulse parameters, focusing on pulse duration, since these two sets of experiments are performed with substantially different pulse durations, 100 ns and 190 fs, respectively. We show that inelastic higher-order effects play a role in the experiment with 100 ns laser pulses (the probed structure is that of the electrolyte solution that is modified by a laser pulse), while in the experiment with 190 fs laser pulses, only the elastic second-order response is measured (probing the unperturbed water structure).
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