Iron force constants of bridgmanite at high pressure: Implications for iron isotope fractionation in the deep mantle

Wang, Wenzhong; Liu, Jiachao; Yang, Hong; Dorfman, Susannah M.; Lv, Mingda; Li, Jie; Zhu, Feng; Zhao, Jiyong; Hu, Michael Y.; Bi, Wenli; Alp, Ercan E.; Xiao, Yuming; Wu, Zhongqing; Lin, Jung-Fu

doi:10.1016/j.gca.2020.11.025

Iron force constants of bridgmanite at high pressure: Implications for iron isotope fractionation in the deep mantle

Journal Article · Thu Dec 03 00:00:00 EST 2020 · Geochimica et Cosmochimica Acta

DOI:https://doi.org/10.1016/j.gca.2020.11.025· OSTI ID:1774970

Wang, Wenzhong ^[1]; Liu, Jiachao ^[2]; Yang, Hong ^[3]; ^[4]; Lv, Mingda ^[4]; Li, Jie ^[5]; Zhu, Feng ^[5]; Zhao, Jiyong ^[6]; Hu, Michael Y. ^[6]; Bi, Wenli ^[7]; Alp, Ercan E. ^[6]; Xiao, Yuming ^[8]; ^[9]; Lin, Jung-Fu ^[10]

Univ. of Science and Technology of China, Hefei (China). Laboratory of Seismology and Physics of Earth’s Interior; Univ. College London (United Kingdom); University of Illinois at Chicago
Univ. of Texas, Austin, TX (United States); Michigan State Univ., East Lansing, MI (United States)
Center for High Pressure Science and Technology Advanced Research (HPSTAR), Pudong, Shanghai (China)
Michigan State Univ., East Lansing, MI (United States)
Univ. of Michigan, Ann Arbor, MI (United States)
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Univ. of Illinois at Urbana-Champaign, IL (United States)
Argonne National Lab. (ANL), Argonne, IL (United States). High Pressure Collaborative Access Team (HPCAT)
Univ. of Science and Technology of China, Hefei (China). Laboratory of Seismology and Physics of Earth’s Interior
Univ. of Texas, Austin, TX (United States)

The isotopic compositions of iron in major mantle minerals may record chemical exchange between deep-Earth reservoirs as a result of early differentiation and ongoing plate tectonics processes. Bridgmanite (Bdg), the most abundant mineral in the Earth’s lower mantle, can incorporate not only Al but also Fe with different oxidation states and spin states, which in turn can influence the distribution of Fe isotopes between Bdg and ferropericlase (Fp) and between the lower mantle and the core. In this study, we combined first-principles calculations with high-pressure nuclear resonant inelastic X-ray scattering measurements to evaluate the effects of Fe site occupancy, valence, and spin states at lower-mantle conditions on the reduced Fe partition function ratio (b-factor) of Bdg. Our results show that the spin transition of octahedral-site (B-site) Fe³⁺ in Bdg under mid-lower-mantle conditions generates a +0.09‰ increase in its b-factor, which is the most significant effect compared to Fe site occupancy and valence. Fe²⁺-bearing Bdg varieties have smaller b-factors relative to Fe³⁺-bearing varieties, especially those containing B-site Fe³⁺. Our models suggest that Fe isotopic fractionation between Bdg and Fp is only significant in the lowermost mantle due to the occurrence of low-spin Fe2+ in Fp. Assuming early segregation of an iron core from a deep magma ocean, we find that neither core formation nor magma ocean crystallization would have resulted in resolvable Fe isotope fractionation. In contrast, Fe isotopic fractionation between low-spin Fe³⁺-bearing Bdg/Fe²⁺-bearing Fp and metallic iron at the core-mantle boundary may have enriched the lowermost mantle in heavy Fe isotopes by up to +0.20‰.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Univ. of Illinois, Chicago, IL (United States)

Sponsoring Organization:: Chinese Academy of Sciences (CAS); National Aeronautic and Space Administration (NASA); National Natural Science Foundation of China (NSFC); National Science Foundation (NSF); USDOE National Nuclear Security Administration (NNSA), Office of Defense Programs (DP); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division

Grant/Contract Number:: AC02-06CH11357; NA0003975

OSTI ID:: 1774970

Alternate ID(s):: OSTI ID: 1797911

Journal Information:: Geochimica et Cosmochimica Acta, Journal Name: Geochimica et Cosmochimica Acta Vol. 294; ISSN 0016-7037

Publisher:: Elsevier; The Geochemical Society; The Meteoritical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Iron force constants of bridgmanite at high pressure: Implications for iron isotope fractionation in the deep mantle

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