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Equation of state and spin crossover of (Mg,Fe)O at high pressure, with implications for explaining topographic relief at the core-mantle boundary

  • Natalia V. Solomatova EMAIL logo , Jennifer M. Jackson , Wolfgang Sturhahn , June K. Wicks , Jiyong Zhao , Thomas S. Toellner , Bora Kalkan and William M. Steinhardt
Published/Copyright: April 30, 2016
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American Mineralogist
From the journal American Mineralogist Volume 101 Issue 5

Abstract

Iron-bearing periclase is thought to represent a significant fraction of Earth’s lower mantle. However, the concentration of iron in (Mg,Fe)O is not well constrained at all mantle depths. Therefore, understanding the effect of iron on the density and elastic properties of this phase plays a major role in interpreting seismically observed complexity in the deep Earth. Here we examine the high-pressure behavior of polycrystalline (Mg,Fe)O containing 48 mol% FeO, loaded hydrostatically with neon as a pressure medium. Using X-ray diffraction and synchrotron Mössbauer spectroscopy, we measure the equation of state to about 83 GPa and hyperfine parameters to 107 GPa at 300 K. A gradual volume drop corresponding to a high-spin (HS) to low-spin (LS) crossover is observed between ~45 and 83 GPa with a volume drop of 1.85% at 68.8(2.7) GPa, the calculated spin transition pressure. Using a newly formulated spin crossover equation of state, the resulting zero-pressure isothermal bulk modulus K0T,HS for the HS state is 160(2) GPa with a K0T,HS′ of 4.12(14) and a V0,HS of 77.29(0) Å3. For the LS state, the K0T,LS is 173(13) GPa with a K0T,LS′ fixed to 4 and a V0,LS of 73.64(94) Å3. To confirm that the observed volume drop is due to a spin crossover, the quadrupole splitting (QS) and isomer shift (IS) are determined as a function of pressure. At low pressures, the Mössbauer spectra are well explained with two Fe2+-like sites. At pressure between 44 and 84, two additional Fe2+-like sites with a QS of 0 are required, indicative of low-spin iron. Above 84 GPa, two low-spin Fe2+-like sites with increasing weight fraction explain the data well, signifying the completion of the spin crossover. To systematically compare the effect of iron on the equation of state parameters for (Mg,Fe)O, a spin crossover equation of state was fitted to the pressure-volume data of previous measurements. Our results show that K0,HS is insensitive to iron concentration between 10 to 60 mol% FeO, while the spin transition pressure and width generally increases from about 50–80 and 2–25 GPa, respectively. A key implication is that iron-rich (Mg,Fe)O at the core-mantle boundary would likely contain a significant fraction of high-spin (less dense) iron, contributing a positive buoyancy to promote observable topographic relief in tomographic images of the lowermost mantle.

Keywords: (Mg,Fe)O; ferropericlase; spin crossover; equation of state; X-ray diffraction; synchrotron Mössbauer spectroscopy; lower mantle; ultralow-velocity zones

Acknowledgments

We thank E.E. Alp and W. Bi for the isomer shift measurement of the reference stainless steel foil. We are thankful to NSF-EAR-CAREER-0956166, NSF-CSEDI-EAR-1161046, and COMPRES, which partially supports operations at Sector 3 (APS), the Mössbauer Laboratory (APS), and Beamline 12.2.2 (ALS). Ambient X-ray diffraction experiments at 11-BM of APS were made possible by Saul Lapidus and Lynn Ribaud. Microprobe analyses at Caltech were partially funded by MRSEX Program of the NSF under DMR-0080065. Ruby fluorescence measurements for the SMS experiments were conducted at GSE-CARS. Use of the Advanced Photon Source is supported by the U.S. DOE, Office of Science (DE-AC02-06CH11357). The Advanced Light Source is supported by the U.S. DOE, Office of Science (DE-AC02-05CH11231). We thank two anonymous reviewers for their thoughtful comments.

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Received: 2015-7-24
Accepted: 2015-12-24
Published Online: 2016-4-30
Published in Print: 2016-5-1

© 2016 by Walter de Gruyter Berlin/Boston

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https://doi.org/10.2138/am-2016-5510
Keywords for this article
(Mg,Fe)O; ferropericlase; spin crossover; equation of state; X-ray diffraction; synchrotron Mössbauer spectroscopy; lower mantle; ultralow-velocity zones

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  44. Compressibility of 2M1 muscovite-paragonite series minerals: A computational study to 6 GPa
  45. Research Article
  46. Joegoldsteinite: A new sulfide mineral (MnCr2S4) from the Social Circle IVA iron meteorite
  47. Research Article
  48. Oxygen isotope thermometry reveals high magmatic temperatures and short residence times in Yellowstone and other hot-dry rhyolites compared to cold-wet systems
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  50. The elastic tensor of monoclinic alkali feldspars
  51. Letter
  52. Ca neighbors from XANES spectroscopy: A tool to investigate structure, redox, and nucleation processes in silicate glasses, melts, and crystals
  53. Letter
  54. Coupled substitution of Fe3+ and H+ for Si in wadsleyite: A study by polarized infrared and Mössbauer spectroscopies and single-crystal X-ray diffraction
  55. Research Article
  56. New Mineral Names
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