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Structural and electron spin state changes in an x-ray heated iron carbonate system at the Earth's lower mantle pressures

  • The determination of the spin state of iron-bearing compounds at high pressure and temperature is crucial for our understanding of chemical and physical properties of the deep Earth. Studies on the relationship between the coordination of iron and its electronic spin structure in iron-bearing oxides, silicates, carbonates, iron alloys, and other minerals found in the Earth's mantle and core are scarce because of the technical challenges to simultaneously probe the sample at high pressures and temperatures. We used the unique properties of a pulsed and highly brilliant x-ray free electron laser (XFEL) beam at the High Energy Density (HED) instrument of the European XFEL to x-ray heat and probe samples contained in a diamond anvil cell. We heated and probed with the same x-ray pulse train and simultaneously measured x-ray emission and x-ray diffraction of an FeCO3 sample at a pressure of 51 GPa with up to melting temperatures. We collected spin state sensitive Fe K beta(1,3) fluorescence spectra and detected the sample's structuralThe determination of the spin state of iron-bearing compounds at high pressure and temperature is crucial for our understanding of chemical and physical properties of the deep Earth. Studies on the relationship between the coordination of iron and its electronic spin structure in iron-bearing oxides, silicates, carbonates, iron alloys, and other minerals found in the Earth's mantle and core are scarce because of the technical challenges to simultaneously probe the sample at high pressures and temperatures. We used the unique properties of a pulsed and highly brilliant x-ray free electron laser (XFEL) beam at the High Energy Density (HED) instrument of the European XFEL to x-ray heat and probe samples contained in a diamond anvil cell. We heated and probed with the same x-ray pulse train and simultaneously measured x-ray emission and x-ray diffraction of an FeCO3 sample at a pressure of 51 GPa with up to melting temperatures. We collected spin state sensitive Fe K beta(1,3) fluorescence spectra and detected the sample's structural changes via diffraction, observing the inverse volume collapse across the spin transition. During x-ray heating, the carbonate transforms into orthorhombic Fe4C3O12 and iron oxides. Incipient melting was also observed. This approach to collect information about the electronic state and structural changes from samples contained in a diamond anvil cell at melting temperatures and above will considerably improve our understanding of the structure and dynamics of planetary and exoplanetary interiors.show moreshow less

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Author details:Johannes M. KaaORCiD, Christian SternemannORCiD, Karen AppelORCiD, Valerio CerantolaORCiD, Thomas R. PrestonORCiD, Christian AlbersORCiD, Mirko ElbersORCiD, Lelia LibonORCiDGND, Mikako Makita, Alexander Pelka, Sylvain PetitgirardORCiD, Christian PlückthunORCiD, Vladimir RoddatisORCiD, Christoph J. SahleORCiD, Georg SpiekermannORCiDGND, Christian SchmidtORCiD, Anja SchreiberORCiD, Robin SakrowskiORCiD, Metin Tolan, Max WilkeORCiD, Ulf ZastrauORCiD, Zuzana KonopkovaORCiD
DOI:https://doi.org/10.1103/PhysRevResearch.4.033042
ISSN:2643-1564
Title of parent work (English):Physical review research
Publisher:American Physical Society
Place of publishing:College Park
Publication type:Article
Language:English
Date of first publication:2022/07/15
Publication year:2022
Release date:2024/06/06
Volume:4
Issue:3
Article number:033042
Number of pages:9
Funding institution:Federal Ministry of Education and Research of Germany [05K19PE2];; Deutsche Forschungsgemeinschaft [AP 262/1-2, KO5262/1]; DFG [1079/4-1,; 1079/2-1, 2000/13-1, 2000/17-1, 2000/8-2, DFG-FOR2125]; ESRF
Organizational units:Mathematisch-Naturwissenschaftliche Fakultät / Institut für Physik und Astronomie
DDC classification:5 Naturwissenschaften und Mathematik / 53 Physik / 530 Physik
Peer review:Referiert
Publishing method:Open Access / Gold Open-Access
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License (German):License LogoCC-BY - Namensnennung 4.0 International
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