Evolution of Chemical Bonding and Spin-Pairing Energy in Ferropericlase across Its Spin Transition

We present a setup exploiting a von Hámos spectrometer in order to study (resonant) X-ray emission of matter exposed to high pressure. The capabilities of this setup are demonstrated for the case of FeO at pressures between 13 GPa and 75 GPa. The setup provides high-quality Kβ 1,3 X-ray emission spectra at high pressures for iron spin state analysis within minutes and iron valence-to-core spectra in less than one hour. Resonant X-ray emission maps can be obtained on a timescale of one hour with 1.0 eV and in approximately 3 hours with 0.2 eV incident energy resolution. Both Kα and Kβ emission can be utilized to gain L-edge and M-edge-like information, respectively, with the option of measuring both simultaneously. The spin state results on FeO between 13 GPa and 75 GPa are in accordance with recent literature. The structural distortion is reflected in both, valence-to-core spectra and resonant X-ray emission maps, which showcase the great potential of the presented setup. The achieved data acquisition times are promising to couple pressure with temperature by laser heating.

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Reduced charge transfer in mixed-spin ferropericlase inferred from its high-pressure refractive index

Schifferle,

Speziale,

Winkler

et al. 2024

American Mineralogist

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Physical properties of mantle minerals are essential for comprehensive geodynamic modelling. High-pressure experiments allow measurements of physical properties but fundamental insights into their evolution with pressure are often experimentally inaccessible.Here we report the first in situ experimental determination of the optical refractive index, its wavelength-dispersion, and optical absorption coefficient of ferropericlase up to ~140 GPa at room temperature. All these properties change gradually in dominantly high-spin (below ~50 GPa) and low-spin (above ~80 GPa) ferropericlase. However, in the mixed-spin state (i.e., significant presence of both high-and low-spin iron), the index dispersion and the absorption coefficient decrease by a factor of three and ~30 %, respectively. These anomalies suggest that charge transport by small polaron is reduced in mixed-spin ferropericlase, providing fundamental insights into the factor-of-three lower electrical conductivity of ferropericlase at ~50-70 GPa.

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Evolution of Chemical Bonding and Spin-Pairing Energy in Ferropericlase across Its Spin Transition

Cited by 3 publications

References 81 publications

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Non-resonant and resonant X-ray emission at high pressure using a von Hámos setup: the case of FeO

Reduced charge transfer in mixed-spin ferropericlase inferred from its high-pressure refractive index

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