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Polyelectrolytes induce water-water correlations that result in dramatic viscosity changes and nuclear quantum effects.


ABSTRACT: Ions interact with water via short-ranged ion-dipole interactions. Recently, an additional unexpected long-ranged interaction was found: The total electric field of ions influences water-water correlations over tens of hydration shells, leading to the Jones Ray effect, a 0.3% surface tension depression. Here, we report such long-range interactions contributing substantially to both molecular and macroscopic properties. Femtosecond elastic second harmonic scattering (fs-ESHS) shows that long-range electrostatic interactions are remarkably strong in aqueous polyelectrolyte solutions, leading to an increase in water-water correlations. This increase plays a role in the reduced viscosity, which changes more than two orders of magnitude with polyelectrolyte concentration. Using D2O instead of H2O shifts both the fs-ESHS and the viscosity curve by a factor of ~10 and reduces the maximum viscosity value by 20 to 300%, depending on the polyelectrolyte. These phenomena cannot be explained using a mean-field approximation of the solvent and point to nuclear quantum effects.

SUBMITTER: Dedic J 

PROVIDER: S-EPMC6989307 | biostudies-literature | 2019 Dec

REPOSITORIES: biostudies-literature

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Polyelectrolytes induce water-water correlations that result in dramatic viscosity changes and nuclear quantum effects.

Dedic J J   Okur H I HI   Roke S S  

Science advances 20191206 12


Ions interact with water via short-ranged ion-dipole interactions. Recently, an additional unexpected long-ranged interaction was found: The total electric field of ions influences water-water correlations over tens of hydration shells, leading to the Jones Ray effect, a 0.3% surface tension depression. Here, we report such long-range interactions contributing substantially to both molecular and macroscopic properties. Femtosecond elastic second harmonic scattering (fs-ESHS) shows that long-rang  ...[more]

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