Snapshots of long-range perturbations in aqueous NaCl solutions

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Fig. 1 Snapshots of long-range perturbations in aqueous NaCl solutions. Snapshots of long-range perturbations in aqueous NaCl solutions. (A) Illustration of two H-bonded water molecules that are orientationally correlated. The black arrows represent different axes along which H-bonds can be broken. fs-ESHS is only sensitive to the breaking of this H-bond via rotation (black curved arrow). Nuclear quantum effects predict that the H-bond bending mode is stronger, whereas the H-bond stretching mode is weaker, for D2O compared to H2O. (B) Sketch of the fs-ESHS experiment. fs-ESHS intensities are recorded at a scattering angle (θ) of 90o. P(S) refers to a polarization direction parallel (perpendicular) to the scattering plane. (C) Top: Illustration of the different regimes probed in the experiment. At low ionic strengths (1), each ion induces long-range structural water correlations in its vicinity, forming a water-ordered domain. At higher ionic strengths, more domains appear. These domains (2) start to overlap and (3) interfere with one another, leading to a saturation of the observed signal. Bottom: fs-ESHS intensities, relative to that of H2O, measured from NaCl solutions. Four different polarization combinations were measured: PoutPinPin, PoutSinSin, SoutPinPin, and SoutSinSin. Only the PoutPinPin and PoutSinSin intensities change with increasing NaCl concentrations. Yixing Chen et al. Sci Adv 2016;2:e1501891 Copyright © 2016, The Authors