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Using first-principles calculations, this study evaluates the structure, equation of state, and elasticity of three compositions of phase D up to 75 GPa: (1) the magnesium endmember [MgSi2O4(OH)2], (2) the aluminum endmember [Al2SiO4(OH)2], and (3) phase D with 50% Al-substitution [AlMg0.5Si1.5O4(OH)2]. We find that the Mg-endmember undergoes hydrogen-bond symmetrization and that this symmetrization is linked to a 22% increase in the bulk modulus of phase D, in agreement with previous studies. Al2SiO4(OH)2 also undergoes hydrogen-bond symmetrization, but the concomitant increase in bulk modulus is only 13%—a significant departure from the 22% increase of the Mg-endmember. Additionally, Al-endmember phase D is denser (2%–6%), less compressible (6%–25%), and has faster compressional (6%–12%) and shear velocities (12%–15%) relative to its Mg-endmember counterpart. Finally, we investigated the properties of phase D with 50% Al-substitution [AlMg0.5Si1.5O4(OH)2], and found that the hydrogen-bond symmetrization, equation of state parameters, and elastic constants of this tie-line composition cannot be accurately modeled by interpolating the properties of the Mg- and Al-endmembers.more » « less
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Thompson, Elizabeth C. ; Campbell, Andrew J. ; Tsuchiya, Jun ( , Geochemistry, Geophysics, Geosystems)
Abstract The stability, structure, and elastic properties of pyrite‐type (FeS2structured) FeO2H were determined using density functional theory‐based computations with an internally consistent Coulombic self‐interaction term (
U eff ). The properties of pyrite‐type FeO2H are compared to that of pyrite‐type AlO2H, with which it likely forms a solid solution at high temperature, as well as the respective lower pressure CaCl2‐type polymorphs of both endmembers:ϵ ‐FeOOH andδ ‐AlOOH. Due to substantial differences in the CaCl2‐type → pyrite‐type structural transition pressures of these endmembers, the stabilities of the (Al,Fe)O2H solid solution polymorphs are anticipated to be compositionally driven at lower mantle pressures. As the geophysical properties of (Al,Fe)OOH are structurally dependant, interpretations regarding the contribution of pyrite‐type FeO2H to seismically observed features must take into account the importance of this broad phase loop. With this in mind, Fe‐rich pyrite‐type (Al,Fe)OOH may coexist with Al‐dominant CaCl2‐typeδ ‐(Al,Fe)OOH in the deep Earth. Furthermore, pyrite‐type (Al0.5–0.6,Fe0.4–0.5)O2H can reproduce the reduced compressional and shear velocities characteristic of seismically observed ultra low velocity zones in the Earth's lowermost mantle while Al‐dominant but Fe‐bearing CaCl2‐typeδ ‐(Al,Fe)OOH may contribute to large low shear velocity provinces.