Structure and Density of H2O‐Rich Mg2SiO4 Melts at High Pressure From Ab Initio Simulations

• Published in: Journal of geophysical research. Solid earth Vol. 125; no. 10
• Main Authors: Yuan, Liang, Steinle‐Neumann, Gerd, Suzuki, Akio
• Format: Journal Article
• Language: English
• Published: 01.10.2020
• Subjects: density; density functional theory; high pressure; hydrous silicate melts; structure
• ISSN: 2169-9313; 2169-9356
• DOI: 10.1029/2020JB020365

Water has a strong effect on silicate melt properties, yet its dissolution mechanism in depolymerized melts, typical for mantle composition, remains poorly understood. Here we report results of first‐principles molecular dynamics simulations for hydrous Mg2SiO4 melts with 6, 16, and 27 wt% H2O at pressure and temperature conditions relevant to the upper mantle and mantle transition zone. The results show that hydrogen bonds not only to the network‐forming cation Si but also to Mg which—nevertheless—remains the most important network modifier. There is no evidence to support the hypothesis based on experimental data that water may cause an increase in melt polymerization for ultramafic magmas; the ratio of non‐bridging oxygen per Si increases with the addition of the oxygen from H2O. The partial molar volume of water is independent on concentration in our simulations which allows us to examine the density of hydrous melt systematically. The critical water content—at which melts are neutrally buoyant compared to the surrounding mantle—is ~4 wt% H2O for a pyrolite composition, much lower than the high water content (>10 wt%) observed in petrological experiments and estimated thermodynamically for low‐degree partial melts formed in the vicinity of the mantle transition zone. Plain Language Summary Geophysical observations indicate abrupt changes in the material properties of the Earth's mantle right below and above the transition zone, at a depth between 410 and 660 km. The existence of low‐velocity and high conductivity layers near this region is often taken as an indication for melting caused by the presence of water. However, the density of such hydrous melts is not well characterized over the relevant pressure‐temperature range. Here we present new simulations on Mg2SiO4 melts with a wide range of water concentrations to address this issue. The water content at which hydrous melts have the same density as the surrounding mantle is about 4 wt%, much lower than the high water content (>10 wt%) estimated for melts occurring in the Earth's mantle, suggesting they cannot experience long‐term gravitational stability in the mantle transition zone and its vicinity. We further find that water does not cause a significant change in melt structure as proposed previously. Key Points We perform ab initio molecular dynamics simulations on Mg2SiO4 melts over a wide range of H2O concentrations We find no evidence for an increase in the degree of melt polymerization with water for ultramafic magmas as proposed previously The critical water content at which hydrous peridotitic melts have the same density as the surrounding mantle is about 4 wt%