Isotope effects on the high pressure viscosity of liquid water measured by differential dynamic microscopy

Abstract

Differential dynamic microscopy is performed in diamond anvil cells to measure the viscosity of water along the 24 °C isotherm to high pressure by the determination of the tracer diffusion coefficient of monodisperse silica spheres of known diameter and the application of the Stokes–Einstein–Sutherland equation. This technique allows liquid samples to be compressed to greater pressure prior to freezing than with other viscometry methods. The highest-pressure measurement was made at 1.67 GPa, considerably deeper into the supercompressed regime than previously reported. The effect of the isotopic composition is investigated with samples of normal water, heavy water, and partially deuterated water. When data below 0.25 GPa are excluded, a free volume model fits the observed viscosities well, yielding a theoretical glass transition density close to that observed in very-high-density amorphous ice. The improved fit above 0.25 GPa coincides with the loss of other anomalous behaviors in liquid water caused by hydrogen bonding and represents a transition to properties closer to those of a simple liquid.