skip to main content

Title: Water Concentration in Single‐Crystal (Al,Fe)‐Bearing Bridgmanite Grown From the Hydrous Melt: Implications for Dehydration Melting at the Topmost Lower Mantle

High‐quality single‐crystals of (Al,Fe)‐bearing bridgmanite, Mg0.88Fe3+0.065Fe2+0.035Al0.14Si0.90O3, of hundreds of micrometer size were synthesized at 24 GPa and 1800 °C in a Kawai‐type apparatus from the starting hydrous melt containing ~6.7 wt% water. Analyses of synthesized bridgmanite using petrographic microscopy, scanning electron microscopy, and transmission electron microscopy show that the crystals are chemically homogeneous and inclusion free in micrometer‐ to nanometer‐spatial resolutions. Nanosecondary ion mass spectrometry (NanoSIMS) analyses on selected platelets show ~1,020(±70) ppm wt water (hydrogen). The high water concentration in the structure of bridgmanite was further confirmed using polarized and unpolarized Fourier‐transform infrared spectroscopy (FTIR) analyses with two pronounced OH‐stretching bands at ~3,230 and ~3,460 cm−1. Our results indicate that lower‐mantle bridgmanite can accommodate relatively high amount of water. Therefore, dehydration melting at the topmost lower mantle by downward flow of transition zone materials would require water content exceeding ~0.1 wt%.

more » « less
Author(s) / Creator(s):
 ;  ;  ;  ;  ;  ;  ;  ;  ;  ;  
Publisher / Repository:
DOI PREFIX: 10.1029
Date Published:
Journal Name:
Geophysical Research Letters
Page Range / eLocation ID:
p. 10346-10357
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract

    Fe‐Al‐bearing bridgmanite may be the dominant host for ferric iron in Earth's lower mantle. Here we report the synthesis of (Mg0.5Fe3+0.5)(Al0.5Si0.5)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) Å3,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.

    more » « less
  2. Abstract

    The thermal conductivity of bridgmanite, the primary constituent of the Earth's lower mantle, has been investigated using diamond anvil cells at pressures up to 85 GPa and temperatures up to 3,100 K. We report the results of time‐domain optical laser flash heating and X‐ray Free Electron Laser heating experiments from a variety of bridgmanite samples with different Al and Fe contents. The results demonstrate that Fe or Fe,Al incorporation in bridgmanite reduces thermal conductivity by about 50% in comparison to end‐member MgSiO3at the pressure‐temperature conditions of Earth's lower mantle. The effect of temperature on the thermal conductivity at 28–60 GPa is moderate, well described as , whereais 0.2–0.5. The results yield thermal conductivity of 7.5–15 W/(m × K) in the thermal boundary layer of the lowermost mantle composed of Fe,Al‐bearing bridgmanite.

    more » « less
  3. Abstract

    The primary phase of the Earth’s lower mantle, (Al, Fe)‐bearing bridgmanite, transitions to the post‐perovskite (PPv) phase at Earth’s deep mantle conditions. Despite extensive experimental and ab initio investigations, there are still important aspects of this transformation that need clarification. Here, we address this transition in (Al3+, Fe3+)‐, (Al3+)‐, (Fe2+)‐, and (Fe3+)‐bearing bridgmanite using ab initio calculations and validate our results against experiments on similar compositions. Consistent with experiments, our results show that the onset transition pressure and the width of the two‐phase region depend distinctly on the chemical composition: (a) Fe3+‐, Al3+‐, or (Al3+, Fe3+)‐alloying increases the transition pressure, while Fe2+‐alloying has the opposite effect; (b) in the absence of coexisting phases, the pressure‐depth range of the Pv‐PPv transition is likely too broad to cause a sharp D” discontinuity (<30 km); (c) the average Clapeyron slope of the two‐phase regions are consistent with previous measurements, calculations in MgSiO3, and inferences from seismic data. In addition, (d) we observe a softening of the bulk modulus in the two‐phase region. The consistency between our results and experiments gives us the confidence to proceed and examine this transition in aggregates with different compositions computationally, which will be fundamental for resolving the most likely chemical composition of the D region by analyses of tomographic images.

    more » « less
  4. 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 higherVP/VSratio 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.

    more » « less
  5. Abstract

    The amount of ferric iron Fe3+in the lower mantle is largely unknown and may be influenced by the disproportionation reaction of ferrous iron Fe2+into metallic Fe and Fe3+triggered by the formation of bridgmanite. Recent work has shown that Fe3+has a strong effect on the density and seismic wave speeds of bridgmanite and the incorporation of impurities such as aluminum. In order to further investigate the effects of ferric iron on mineral behavior at lower mantle conditions, we conducted laser‐heated diamond‐anvil cell (LHDAC) experiments on two sets of samples nearly identical in composition (an aluminum‐rich pyroxenite glass) except for the Fe3+content; with one sample with more Fe3+(“oxidized”: Fe3+/ΣFe ~ 55%) and the other with less Fe3+(“reduced”: Fe3+/ΣFe ~ 11%). We heated the samples to lower mantle conditions, and the resulting assemblages were drastically different between the two sets of samples. For the reduced composition, we observed a multiphase assemblage dominated by bridgmanite and calcium perovskite. In contrast, the oxidized material yielded a single phase of Ca‐bearing bridgmanite. These Al‐rich pyroxenite samples show a difference in density and seismic velocities for these two redox states, where the reduced assemblage is denser than the oxidized assemblage by ~1.5% at the bottom of the lower mantle and slower (bulk sound speed) by ~2%. Thus, heterogeneities of Fe3+content may lead to density and seismic wave speed heterogeneities in Earth's lower mantle.

    more » « less