TY - JOUR
T1 - Comment on "water-water correlations in electrolyte solutions probed by hyper-Rayleigh scattering" [J. Chem. Phys. 147, 214505 (2017)]
AU - Chen, Y.
AU - Okur, H. I.
AU - Dupertuis, N.
AU - Dedic, J.
AU - Wilkins, D. M.
AU - Ceriotti, M.
AU - Roke, S.
PY - 2018/10/28
Y1 - 2018/10/28
N2 - 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).
AB - 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).
UR - http://www.scopus.com/inward/record.url?scp=85055906635&partnerID=8YFLogxK
U2 - 10.1063/1.5023579
DO - 10.1063/1.5023579
M3 - Article
C2 - 30384715
AN - SCOPUS:85055906635
VL - 149
JO - Journal of Chemical Physics
JF - Journal of Chemical Physics
SN - 0021-9606
IS - 16
M1 - 167101
ER -