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Title: Electronic spin state of iron in lower mantle perovskite

Journal Article · · Proc. Natl. Acad. Sci. USA
OSTI ID:1008729

The electronic spin state of iron in lower mantle perovskite is one of the fundamental parameters that governs the physics and chemistry of the most voluminous and massive shell in the Earth. We present experimental evidence for spin-pairing transition in aluminum-bearing silicate perovskite (Mg,Fe)(Si,Al)O{sub 3} under the lower mantle pressures. Our results demonstrate that as pressure increases, iron in perovskite transforms gradually from the initial high-spin state toward the final low-spin state. At 100 GPa, both aluminum-free and aluminum-bearing samples exhibit a mixed spin state. The residual magnetic moment in the aluminum-bearing perovskite is significantly higher than that in its aluminum-free counterpart. The observed spin evolution with pressure can be explained by the presence of multiple iron species and the occurrence of partial spin-paring transitions in the perovskite. Pressure-induced spin-pairing transitions in the perovskite would have important bearing on the magnetic, thermoelastic, and transport properties of the lower mantle, and on the distribution of iron in the Earth's interior. The lower mantle constitutes more than half of the Earth's interior by volume (1), and it is believed to consist predominantly (80-100%) of (Mg,Fe)(Si,Al)O{sub 3} perovskite (hereafter called perovskite), with up to 20% (Mg,Fe)O ferropericlase (2). The electronic spin state of iron has direct influence on the physical properties and chemical behavior of its host phase. Hence, knowledge on the spin state of iron is important for the interpretation of seismic observations, geochemical modeling, and geodynamic simulation of the Earth's deep interior (3, 4). Crystal field theory (4, 5) and band theory (6) predicted that a high-spin to low-spin transition would occur as a result of compression. To date, no experimental data exist on the spin sate of iron in Al-bearing perovskite. To detect possible spinpairing transition of iron in perovskite under the lower mantle conditions, we measured the x-ray emission spectra of an Al-bearing perovskite sample to 100 GPa. For comparison, a parallel measurement was also carried out on an Al-free perovskite sample.

Research Organization:
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Organization:
USDOE
OSTI ID:
1008729
Journal Information:
Proc. Natl. Acad. Sci. USA, Vol. 101, Issue (39) ; 09, 2004; ISSN 0027-8424
Country of Publication:
United States
Language:
ENGLISH