Densification mechanisms of haplogranite glasses as a function of water content and pressure based on density and Raman data

This study investigates the effect of pressure (1 atm-2.5 GPa) and water (0.15, 2.7, 3.6 and 5.2 wt% H2O) on the network structure of alkali-rich alumino-silicate glasses synthesized at 1000 °C. Density increases linearly with pressure in the water-poor composition, while in the water-rich glasses and above 1.5 GPa densification decreases with pressure. Raman data suggest that several structural changes follow one upon another with increasing pressure and water content. The almost dry glasses undergo large modifications of the network ring structure with pressure, namely a decrease in average T-O-T angle, change in ring size statistics and possibly an increasingly homogeneous distribution of Al- and Si-rich domains at high pressure. Water dissolution favors a homogenization of ring sizes at low pressures. Pressure essentially induces a decrease in the average intertetrahedral angle and, above 1.5 GPa, a possible redistribution of Al/Si-rich regions. Pressure induces an increase in O-H bonding but decreases the O-H bond strength. The observed structural modifications are consistent with the decreasing net effect of pressure on viscosity as temperature and water increase through variation of the activation volume of viscosity.