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1. Formation of large low shear velocity provinces through the decomposition of oxidized mantle

   https://doi.org/10.1038/s41467-021-22185-1  

   Wang, Wenzhong; Liu, Jiachao; Zhu, Feng; Li, Mingming; Dorfman, Susannah M.; Li, Jie; Wu, Zhongqing (March 2021, Nature Communications)

   Abstract Large Low Shear Velocity Provinces (LLSVPs) in the lowermost mantle are key to understanding the chemical composition and thermal structure of the deep Earth, but their origins have long been debated. Bridgmanite, the most abundant lower-mantle mineral, can incorporate extensive amounts of iron (Fe) with effects on various geophysical properties. Here our high-pressure experiments and ab initio calculations reveal that a ferric-iron-rich bridgmanite coexists with an Fe-poor bridgmanite in the 90 mol% MgSiO₃–10 mol% Fe₂O₃system, rather than forming a homogeneous single phase. The Fe³⁺-rich bridgmanite has substantially lower velocities and a higherV_P/V_Sratio than MgSiO₃bridgmanite under lowermost-mantle conditions. Our modeling shows that the enrichment of Fe³⁺-rich bridgmanite in a pyrolitic composition can explain the observed features of the LLSVPs. The presence of Fe³⁺-rich materials within LLSVPs may have profound effects on the deep reservoirs of redox-sensitive elements and their isotopes. 

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2. High Sodium Solubility in Magnesiowüstite in Iron‐Rich Deep Lower Mantle

   https://doi.org/10.1029/2023GC011390  

   Dorfman, Susannah_M; Hsu, Han; Nabiei, Farhang; Cantoni, Marco; Badro, James; Prakapenka, Vitali_B (June 2024, Geochemistry, Geophysics, Geosystems)

   Abstract (Mg,Fe)O ferropericlase‐magnesiowüstite has been proposed to host the majority of Earth's sodium, but the mechanism and capacity for incorporating the alkali cation remain unclear. In this work, experiments in the laser‐heated diamond anvil cell and first‐principles calculations determine the solubility of sodium and favorability of sodium incorporation in iron‐rich magnesiowüstite relative to (Mg,Fe)SiO₃bridgmanite. Reaction of Mg/(Mg + Fe) (Mg#) 55 and 28 olivine with NaCl at 33–128 GPa and 1600–3000 K produces iron‐rich magnesiowüstite containing several percent sodium, while iron‐rich bridgmanite contains little to no detectable sodium. In sodium‐saturated magnesiowüstite, sodium number [Na/(Na + Mg + Fe)] is 2–5 atomic percent at pressures below 60 GPa and drastically increases to 10–20 atomic percent at deep lower mantle pressures. For these two compositions, there is no significant dependence of the results on Mg#. Our calculations not only show consistent results with experiments but further indicate that such an increase in solubility and partitioning of Na into magnesiowüstite is driven by the spin transition in iron. These results provide fundamental constraints on the crystal chemistry of sodium at lower‐mantle conditions. If the sodium capacity of (Mg,Fe)O is not strongly dependent on Mg#, (Mg,Fe)O in the lower mantle may have the capacity to store the entire sodium budget of the Earth. 

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3. Synthesis, Elasticity, and Spin State of an Intermediate MgSiO ₃ ‐FeAlO ₃ Bridgmanite: Implications for Iron in Earth's Lower Mantle

   https://doi.org/10.1029/2020JB019964  

   Zhu, Feng; Liu, Jiachao; Lai, Xiaojing; Xiao, Yuming; Prakapenka, Vitali; Bi, Wenli; Alp, E. Ercan; Dera, Przemyslaw; Chen, Bin; Li, Jie (July 2020, Journal of Geophysical Research: Solid Earth)

   Abstract Fe‐Al‐bearing bridgmanite may be the dominant host for ferric iron in Earth's lower mantle. Here we report the synthesis of (Mg_0.5Fe³⁺_0.5)(Al_0.5Si_0.5)O₃bridgmanite (FA50) with the highest Fe³⁺‐Al³⁺coupled substitution known to date. X‐ray diffraction measurements showed that at ambient conditions, the FA50 adopted the LiNbO₃structure. Upon compression at room temperature to 18 GPa, it transformed back into the bridgmanite structure, which remained stable up to 102 GPa and 2,600 K. Fitting Birch‐Murnaghan equation of state of FA50 bridgmanite yieldsV₀ = 172.1(4) ų,K₀ = 229(4) GPa withK₀′ = 4(fixed). The calculated bulk sound velocity of the FA50 bridgmanite is ~7.7% lower than MgSiO₃bridgmanite, mainly because the presence of ferric iron increases the unit‐cell mass by 15.5%. This difference likely represents the upper limit of sound velocity anomaly introduced by Fe³⁺‐Al³⁺substitution. X‐ray emission and synchrotron Mössbauer spectroscopy measurements showed that after laser annealing, ~6% of Fe³⁺cations exchanged with Al³⁺and underwent the high‐ to low‐spin transition at 59 GPa. The low‐spin proportion of Fe³⁺increased gradually with pressure and reached 17–31% at 80 GPa. Since the cation exchange and spin transition in this Fe³⁺‐Al³⁺‐enriched bridgmanite do not cause resolvable unit‐cell volume reduction, and the increase of low‐spin Fe³⁺fraction with pressure occurs gradually, the spin transition would not produce a distinct seismic signature in the lower mantle. However, it may influence iron partitioning and isotopic fractionation, thus introducing chemical heterogeneity in the lower mantle. 

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4. Composition and Pressure Effects on Partitioning of Ferrous Iron in Iron-Rich Lower Mantle Heterogeneities

   https://doi.org/10.3390/min11050512  

   Dorfman, Susannah M.; Nabiei, Farhang; Boukaré, Charles-Edouard; Prakapenka, Vitali B.; Cantoni, Marco; Badro, James; Gillet, Philippe (May 2021, Minerals)

   Both seismic observations of dense low shear velocity regions and models of magma ocean crystallization and mantle dynamics support enrichment of iron in Earth’s lowermost mantle. Physical properties of iron-rich lower mantle heterogeneities in the modern Earth depend on distribution of iron between coexisting lower mantle phases (Mg,Fe)O magnesiowüstite, (Mg,Fe)SiO3 bridgmanite, and (Mg,Fe)SiO3 post-perovskite. The partitioning of iron between these phases was investigated in synthetic ferrous-iron-rich olivine compositions (Mg0.55Fe0.45)2SiO4 and (Mg0.28Fe0.72)2SiO4 at lower mantle conditions ranging from 33–128 GPa and 1900–3000 K in the laser-heated diamond anvil cell. The resulting phase assemblages were characterized by a combination of in situ X-ray diffraction and ex situ transmission electron microscopy. The exchange coefficient between bridgmanite and magnesiowüstite decreases with pressure and bulk Fe# and increases with temperature. Thermodynamic modeling determines that incorporation and partitioning of iron in bridgmanite are explained well by excess volume associated with Mg-Fe exchange. Partitioning results are used to model compositions and densities of mantle phase assemblages as a function of pressure, FeO-content and SiO2-content. Unlike average mantle compositions, iron-rich compositions in the mantle exhibit negative dependence of density on SiO2-content at all mantle depths, an important finding for interpretation of deep lower mantle structures. 

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5. Partitioning of Iron Between (Mg,Fe)SiO ₃ Liquid and Bridgmanite

   https://doi.org/10.1029/2023GL107979  

   Dragulet, Francis; Stixrude, Lars (June 2024, Geophysical Research Letters)

   Abstract The evolution of the magma ocean that occupied the early Earth is influenced by the buoyancy of crystals in silicate liquid. At lower mantle pressures, silicate crystals are denser than the iso‐chemical liquid, but heavy elements like iron can cause crystals to float if they partition into the liquid phase. Crystal flotation allows for a basal magma ocean, which might explain geochemical anomalies in mantle‐derived magmas, seismic anomalies in the lower mantle, and the source of the Earth's early magnetic field. To examine whether a basal magma ocean is gravitationally stable, we investigate the degree of iron partitioning between (Mg,Fe)SiO₃liquid and bridgmanite. By utilizing ab initio molecular dynamics simulations coupled with thermodynamic integration, we find that iron partitions into the liquid, and increasingly so with increasing pressure. Bridgmanite crystals are found to be buoyant at lower mantle conditions, stabilizing the basal magma ocean. 

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