First-principles study of intermediate-spin ferrous iron in the Earth's lower mantle

Han Hsu, Renata M. Wentzcovitch

研究成果: 雜誌貢獻期刊論文同行評審

29 引文 斯高帕斯(Scopus)


Spin crossover of iron is of central importance in solid Earth geophysics. It impacts all physical properties of minerals that altogether constitute ∼95 vol% of the Earth's lower mantle: ferropericlase [(Mg,Fe)O] and Fe-bearing magnesium silicate (MgSiO3) perovskite. Despite great strides made in the past decade, the existence of an intermediate-spin (IS) state in ferrous iron (Fe2+) (with total electron spin S=1) 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 U (DFT+Usc) calculations, we investigate all possible types of IS states of Fe2+ in (Mg,Fe)O and (Mg,Fe)SiO3 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 Fe2+ is highly unlikely in the Earth's lower mantle.

期刊Physical Review B - Condensed Matter and Materials Physics
出版狀態已出版 - 18 11月 2014


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