scholarly journals Temperature dependence of water-water and ion-water correlations in bulk water and electrolyte solutions probed by femtosecond elastic second harmonic scattering

2018 ◽  
Vol 148 (22) ◽  
pp. 222835 ◽  
Author(s):  
Yixing Chen ◽  
Nathan Dupertuis ◽  
Halil I. Okur ◽  
Sylvie Roke
Keyword(s):  
Temperature Dependence ◽  
Second Harmonic ◽  
Electrolyte Solutions ◽  
Bulk Water ◽  
Second Harmonic Scattering

scholarly journals Electrolytes induce long-range orientational order and free energy changes in the H-bond network of bulk water

2016 ◽  
Vol 2 (4) ◽  
pp. e1501891 ◽  
Author(s):  
Yixing Chen ◽  
Halil I. Okur ◽  
Nikolaos Gomopoulos ◽  
Carlos Macias-Romero ◽  
Paul S. Cremer ◽  
...  
Keyword(s):  
Surface Tension ◽  
Hydrogen Bond ◽  
Second Harmonic ◽  
Orientational Order ◽  
Electrolyte Solutions ◽  
Bulk Water ◽  
Atomic Scale ◽  
Dipole Orientation ◽  
Hydrogen Bond Interactions ◽  
Bond Network

Electrolytes interact with water in many ways: changing dipole orientation, inducing charge transfer, and distorting the hydrogen-bond network in the bulk and at interfaces. Numerous experiments and computations have detected short-range perturbations that extend up to three hydration shells around individual ions. We report a multiscale investigation of the bulk and surface of aqueous electrolyte solutions that extends from the atomic scale (using atomistic modeling) to nanoscopic length scales (using bulk and interfacial femtosecond second harmonic measurements) to the macroscopic scale (using surface tension experiments). Electrolytes induce orientational order at concentrations starting at 10 μM that causes nonspecific changes in the surface tension of dilute electrolyte solutions. Aside from ion-dipole interactions, collective hydrogen-bond interactions are crucial and explain the observed difference of a factor of 6 between light water and heavy water.

scholarly journals Hyaluronan orders water molecules in its nanoscale extended hydration shells

2021 ◽  
Vol 7 (10) ◽  
pp. eabf2558
Author(s):  
J. Dedic ◽  
H. I. Okur ◽  
S. Roke
Keyword(s):  
Second Harmonic ◽  
Hydration Shell ◽  
Water Molecules ◽  
Temperature Dependent ◽  
Flexible Chain ◽  
Optical Modeling ◽  
Hydration Shells ◽  
Second Harmonic Scattering ◽  
Nuclear Quantum Effects ◽  
Extracellular Environment

Hyaluronan (HA) is an anionic, highly hydrated bio-polyelectrolyte found in the extracellular environment, like the synovial fluid between joints. We explore the extended hydration shell structure of HA in water using femtosecond elastic second-harmonic scattering (fs-ESHS). HA enhances orientational water-water correlations. Angle-resolved fs-ESHS measurements and nonlinear optical modeling show that HA behaves like a flexible chain surrounded by extended shells of orientationally correlated water. We describe several ways to determine the concentration-dependent size and shape of a polyelectrolyte in water, using the amount of water oriented by the polyelectrolyte charges as a contrast agent. The spatial extent of the hydration shell is determined via temperature-dependent measurements and can reach up to 475 nm, corresponding to a length of 1600 water molecules. A strong isotope effect, stemming from nuclear quantum effects, is observed when light water (H2O) is replaced by heavy water (D2O), amounting to a factor of 4.3 in the scattered SH intensity.

scholarly journals Second-Harmonic Scattering as a Probe of Structural Correlations in Liquids

2016 ◽  
Vol 7 (21) ◽  
pp. 4311-4316 ◽  
Author(s):  
Gabriele Tocci ◽  
Chungwen Liang ◽  
David M. Wilkins ◽  
Sylvie Roke ◽  
Michele Ceriotti
Keyword(s):  
Second Harmonic ◽  
Second Harmonic Scattering

Optical second-harmonic scattering in rat-tail tendon

Biopolymers ◽  
1981 ◽  
Vol 20 (6) ◽  
pp. 1271-1290 ◽  
Author(s):  
Shmuel Roth ◽  
Isaac Freund
Keyword(s):  
Second Harmonic ◽  
Second Harmonic Scattering ◽  
Tail Tendon ◽  
Rat Tail

What Does Second-Harmonic Scattering Measure in Diluted Electrolytes?

2018 ◽  
Vol 9 (13) ◽  
pp. 3698-3702 ◽  
Author(s):  
Daniel Borgis ◽  
Luc Belloni ◽  
Maximilien Levesque
Keyword(s):  
Second Harmonic ◽  
Second Harmonic Scattering
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