Tetrahedral occupancy of ferric iron in (Mg,Fe)O: Implications for point defects in the Earth's lower mantle

Details Tetrahedral occupancy of ferric iron in (Mg,Fe)O: Implications for point defects in the Earth's lower mantle Tetrahedral occupancy of ferric iron in (Mg,Fe)O: Implications for point defects in the Earth's lower mantle

Jun 2010

adsabs.harvard.edu/cgi-bin/nph-data_query?bibcode=2010pepi..180..179o&link_type=abstract

Physics of the Earth and Planetary Interiors, Volume 180, Issue 3-4, p. 179-188.

Physics

2

Scientific paper

We investigated the concentration and site occupation of ferric iron (Fe3+) in (Mg,Fe)O to understand the influence of point defects on transport properties such as atomic diffusion, electrical conductivity and viscosity. We conducted Mössbauer spectroscopy of (Mg0.8Fe0.2)O single crystals synthesized at temperatures from 1673 to 2273 K and pressures from 5 to 15 GPa with Re-ReO2 and Mo-MoO2 oxygen fugacity buffers. The isomer shift of the Mössbauer spectra suggests that Fe3+ occupies mostly the tetrahedral site at reduced conditions and both the octahedral and tetrahedral sites at oxidized conditions. We formulate a thermodynamic model of point defect dissolution in (Mg,Fe)O which suggests that unassociated tetrahedral Fe3+ is more stable than unassociated octahedral Fe3+ at high-pressure and low oxygen fugacity due to the effect of configurational entropy. The pressure dependence of Fe3+ concentration indicates a change in the dominant site occupancy of Fe3+: (1) Fe3+ in the tetrahedral site, (2) Fe3+ in the octahedral site, and (3) defect clusters of Fe3+ and cation vacancy, in the order of increasing oxygen fugacity and decreasing pressure. This is in reasonable agreement with previously reported experiments on Fe3+ concentration, Mg-Fe interdiffusivity and electrical conductivity. We consider it plausible that (Mg,Fe)O accommodates Fe3+ in the tetrahedral site down to the lower mantle. Based on our results and available experimental data, we discuss the solubility competition between Fe3+ and protons (H+), and its implications for transport properties in the lower mantle.

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