In Situ Raman Spectroscopy and DFT Studies of the Phase Transition from Zircon to Reidite at High P–T Conditions

Zircon (ZrSiO4) provides a good pressure-holding environment for ultra-high-pressure metamorphic minerals during crust exhumation due to its high incompressibility and chemical stability. At high pressure, the zircon can transform to reidite. Previous studies show much higher phase-transition pressures at room temperature than those at high temperature (>1000 K) due to kinetic hindrance. To further investigate the kinetics of the zircon–reidite phase transition at relatively low temperatures, the phase boundary at 298–800 K was determined using a diamond anvil cell combined with in situ Raman spectra. The results show that reidite becomes thermodynamically more stable compared with zircon at 8 GPa at room temperature, and the slope of the phase boundary at 298–800 K abruptly differs from that of previous studies at 1100–1900 K. Compared with the equilibrium phase boundary calculated by the density functional theory, it indicates that the kinetic effect of the zircon–reidite phase transition is obvious, and there exists a sufficiently large energy driving force provided by an overpressure to overcome the activation energy barrier below a critical temperature of approximately 880 K. The temperature dependence of overpressure is about 0.023 GPa/K