Abstract
Spin crossover of iron is of central importance in solid Earth geophysics. It impacts all physical properties of minerals that altogether constitute vol% of the Earth's lower mantle: ferropericlase [(Mg,Fe)O] and Fe-bearing magnesium silicate perovskite. Despite great strides made in the past decade, the existence of an intermediate-spin (IS) state in ferrous iron (with total electron spin and its possible role in the pressure-induced spin crossover in these lower-mantle minerals still remain controversial. Using density functional theory self-consistent Hubbard calculations, we investigate all possible types of IS states of in (Mg,Fe)O and (Mg,Fe) perovskite. Among the possible IS states in these minerals, the most probable IS state has an electronic configuration that significantly reduces the electron overlap and the iron nuclear quadrupole splitting (QS). These most probable IS states, however, are still energetically disfavored, and their QSs are inconsistent with Mössbauer spectra. We therefore conclude that IS is highly unlikely in the Earth's lower mantle.
1 More- Received 23 June 2014
DOI:https://doi.org/10.1103/PhysRevB.90.195205
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