Melting behavior of SiO2 up to 120 GPa

Abstract

The structure of liquid silicates is commonly described as a statistical mixture of various atomic entities with relative abundances that can vary with pressure, temperature and composition. Unfortunately, this view remains largely theoretical due to scarce experimental reports on the silicate melt structure, in particular under pressure. We performed X-ray diffraction of the SiO2 end-member to probe the melting curve up to ~120 GPa and 7000 K, and the melt structure up to ~80 GPa. We confirm the steep increase of the melting curve above ~14 GPa when stishovite becomes stable over coesite in subsolidus conditions, with a slope of about 80 K/GPa. Then, around 45 GPa and 5400 K, the melting curve flattens significantly, an effect most likely reflecting the densification of the SiO2 melt structure. The signal of diffuse X-ray scattering is compatible with a change of the Si coordination number from 4 to 6 along the melting curve, in agreement with previous works reporting a similar evolution during the cold compression of SiO2-glass. Because of the limited pressure range (within 10 to 20 GPa) in which the melting curve changes its slope, we speculate a difficult coexistence of tetrahedral SiO4 and octahedral SiO6 units in SiO2 melt at high pressures.