Abstract
The D” layer at the base of the Earth’s mantle exhibits anomalous seismic properties, which are attributed to heat loss from and chemical interaction with the underlying molten Fe-rich outer core. Here we show that mass transfer due to temperature variations within the D” layer could lead to resolvable fractionation of iron isotopes. We constrain the degree of isotope fractionation by experiments on core-forming Fe alloy liquids at 2100–2300 K and 2 GPa, which demonstrate that heavy Fe isotopes preferentially migrate towards lower temperature and vice versa. We find that this isotope fractionation occurs rapidly due to the high mobility of iron, which reaches 0.013 ± 0.002‰ (2σ) per degree per amu at steady state. Numerical simulations of mantle convection capturing the evolution of a basal thermal boundary layer show that iron isotope fractionation immediately above the core–mantle boundary can reach measurable levels on geologic timescales and that plumes can entrain this fractionated material into the convecting mantle. We suggest that such a process may contribute to the heavy Fe isotope composition of the upper mantle inferred from mantle melts (basalts) and residues (peridotites) relative to chondrites. That being the case, non-traditional stable isotope systems such as Fe may constrain the interactions between the core and mantle.
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Data availability
All data generated during this study are included in this article and its supplementary information and supplementary data files.
Code availability
The version of ASPECT we used to compute the geodynamic models is available online (https://github.com/jdannberg/aspect/commits/iron_fractionation), and all input files required to reproduce our computations, together with instructions for how to run them, are provided in a separate repository (https://github.com/jdannberg/SI-data-thermodiffusion).
References
Boehler, R., Chopelas, A. & Zerr, A. Temperature and chemistry of the core–mantle boundary. Chem. Geol. 120, 199–205 (1995).
Lay, T., Hernlund, J., Garnero, E. J. & Thorne, M. A post-perovskite lens and D” heat flux beneath the central Pacific. Science 314, 1272–1276 (2006).
Kawai, K. & Tsuchiya, T. Temperature profile in the lowermost mantle from seismological and mineral physics joint modeling. Proc. Natl Acad. Sci. USA 106, 22119–22123 (2009).
Brown, S. P., Thorne, M. S., Miyagi, L. & Rost, S. A compositional origin to ultralow-velocity zones. Geophys. Res. Lett. 42, 1039–1045 (2015).
Knittle, E. & Jeanloz, R. Earth’s core–mantle boundary: results of experiments at high pressures and temperatures. Science 251, 1438–1443 (1991).
Williams, Q. & Garnero, E. J. Seismic evidence for partial melt at the base of Earth’s mantle. Science 273, 1528–1530 (1996).
Lay, T., Garnero, E. J. & Williams, Q. Partial melting in a thermo-chemical boundary layer at the base of the mantle. Phys. Earth Planet. Inter. 146, 441–467 (2004).
Zhang, Z. et al. Primordial metallic melt in the deep mantle. Geophys. Res. Lett. 43, 3693–3699 (2016).
Hayden, L. A. & Watson, E. B. A diffusion mechanism for core–mantle interaction. Nature 450, 709–711 (2007).
Crispin, K. L., Saha, S., Morgan, D. & Van Orman, J. A. Diffusion of transition metals in periclase by experiment and first-principles, with implications for core–mantle equilibration during metal percolation. Earth Planet. Sci. Lett. 357–358, 42–53 (2012).
Poirier, J.-P. Core-infiltrated mantle and the nature of the D” layer. J. Geomagn. Geoelectr. 45, 1221–1227 (1993).
Goarant, F., Guyot, F., Peyronneau, J. & Poirier, J.-P. High‐pressure and high‐temperature reactions between silicates and liquid iron alloys, in the diamond anvil cell, studied by analytical electron microscopy. J. Geophys. Res. 97, 4477–4487 (1992).
Shi, C. Y. et al. Formation of an interconnected network of iron melt at Earth’s lower mantle conditions. Nat. Geosci. 6, 971–975 (2013).
Otsuka, K. & Karato, S.-I. Deep penetration of molten iron into the mantle caused by a morphological instability. Nature 492, 243–246 (2012).
Kanda, R. V. S. & Stevenson, D. J. Suction mechanism for iron entrainment into the lower mantle. Geophys. Res. Lett. 33, L02310 (2006).
Jones, T. D., Davies, D. R. & Sossi, P. A. Tungsten isotopes in mantle plumes: heads it’s positive, tails it’s negative. Earth Planet. Sci. Lett. 506, 255–267 (2019).
Humayun, M. Geochemical evidence for excess iron in the mantle beneath Hawaii. Science 306, 91–94 (2004).
Brandon, A. D. & Walker, R. J. The debate over core–mantle interaction. Earth Planet. Sci. Lett. 232, 211–225 (2005).
Bouhifd, M. A., Jephcoat, A. P., Heber, V. S. & Kelley, S. K. N. Helium in Earth’s early core. Nat. Geosci. 6, 982–986 (2013).
Mundl, A. et al. Tungsten-182 heterogeneity in modern ocean island basalts. Science 356, 66–69 (2017).
Rizo, H. et al. 182W evidence for core–mantle interaction in the source of mantle plumes. Geochem. Perspect. Lett. 11, 6–11 (2019).
Konter, J. G. et al. Unusual δ56Fe values in Samoan rejuvenated lavas generated in the mantle. Earth Planet. Sci. Lett. 450, 221–232 (2016).
Poitrasson, F., Halliday, A. N., Lee, D.-C., Levasseur, S. & Teutsch, N. Iron isotope differences between Earth, Moon, Mars and Vesta as possible records of contrasted accretion mechanisms. Earth Planet. Sci. Lett. 223, 253–266 (2004).
Williams, H. M. et al. Fractionation of oxygen and iron isotopes by partial melting processes: implications for the interpretation of stable isotope signatures in mafic rocks. Earth Planet. Sci. Lett. 283, 156–166 (2009).
Williams, H. M. Iron isotope fractionation and the oxygen fugacity of the mantle. Science 304, 1656–1659 (2004).
Williams, H. M. & Bizimis, M. Iron isotope tracing of mantle heterogeneity within the source regions of oceanic basalts. Earth Planet. Sci. Lett. 404, 396–407 (2014).
Craddock, P. R., Warren, J. M. & Dauphas, N. Abyssal peridotites reveal the near-chondritic Fe isotopic composition of the Earth. Earth Planet. Sci. Lett. 365, 63–76 (2013).
Sossi, P. A., Nebel, O. & Foden, J. Iron isotope systematics in planetary reservoirs. Earth Planet. Sci. Lett. 452, 295–308 (2016).
Poitrasson, F., Roskosz, M. & Corgne, A. No iron isotope fractionation between molten alloys and silicate melt to 2000 °C and 7.7 GPa: experimental evidence and implications for planetary differentiation and accretion. Earth Planet. Sci. Lett. 278, 376–385 (2009).
Hin, R. C. & Schmidt, M. W. & Bourdon, B. Experimental evidence for the absence of iron isotope fractionation between metal and silicate liquids at 1 GPa and 1250–1300 °C and its cosmochemical consequences. Geochim. Cosmochim. Acta 93, 164–181 (2012).
Shahar, A. et al. Sulfur-controlled iron isotope fractionation experiments of core formation in planetary bodies. Geochim. Cosmochim. Acta 150, 253–264 (2015).
Elardo, S. M. & Shahar, A. Non-chondritic iron isotope ratios in planetary mantles as a result of core formation. Nat. Geosci. 10, 317–321 (2017).
Liu, J. et al. Iron isotopic fractionation between silicate mantle and metallic core at high pressure. Nat. Commun. 8, 14377 (2017).
Kyser, T. K., Lesher, C. E. & Walker, D. The effects of liquid immiscibility and thermal diffusion on oxygen isotopes in silicate liquids. Contrib. Mineral. Petrol. 133, 373–381 (1998).
Richter, F. M. et al. Isotopic fractionation of the major elements of molten basalt by chemical and thermal diffusion. Geochim. Cosmochim. Acta 73, 4250–4263 (2009).
Huang, F. et al. Isotope fractionation in silicate melts by thermal diffusion. Nature 464, 396–400 (2010).
Brenan, J. M. & Bennett, N. Soret separation of highly siderophile elements in Fe–Ni–S melts: implications for solid metal–liquid metal partitioning. Earth Planet. Sci. Lett. 298, 299–305 (2010).
Dobson, D. P. Self-diffusion in liquid Fe at high pressure. Phys. Earth Planet. Inter. 130, 271–284 (2002).
Lacks, D. J. et al. Isotope fractionation by thermal diffusion in silicate melts. Phys. Rev. Lett. 108, 065901 (2012).
Kincaid, J. M., Cohen, E. G. D. & de Haro, M. L. The Enskog theory for multicomponent mixtures. IV. Thermal diffusion. J. Chem. Phys. 86, 963–975 (1998).
Alfè, D. & Kresse, G. Structure and dynamics of liquid iron under Earth’s core conditions. Phys. Rev. B 61, 132–142 (2000).
Buffett, B. A. & Seagle, C. T. Stratification of the top of the core due to chemical interactions with the mantle. J. Geophys. Res. 115, B04407 (2010).
Morgan, J. P., Hasenclever, J. & Shi, C. New observational and experimental evidence for a plume-fed asthenosphere boundary layer in mantle convection. Earth Planet. Sci. Lett. 366, 99–111 (2013).
Heister, T., Dannberg, J., Gassmöller, R. & Bangerth, W. High accuracy mantle convection simulation through modern numerical methods—II: realistic models and problems. Geophys. J. Int. 210, 833–851 (2017).
Bangerth, W. et al. ASPECT: Advanced Solver for Problems in Earth’s ConvecTion, User Manual Computational Infrastructure for Geodynamics https://aspect.geodynamics.org (accessed 11 February 2020).
Acknowledgements
This work was supported by NSF EAR-1019887 and the Danish National Research Foundation–Niels Bohr Professorship (26-123/8) to C.E.L., by NSF EAR-1250331 to D.J.L. and NSERC Discovery Grants to J.M.B. J.D. was partially supported by the Computational Infrastructure for Geodynamics initiative through NSF EAR-0949446, NSF EAR-1550901 and the Deep Carbon Observatory. The authors acknowledge the Texas Advanced Computing Center, University of Texas at Austin, for providing high-performance computing resources. We thank P. Sossi for very constructive comments and suggestions that helped improve the presentation.
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This project was conceived and managed by C.E.L. N.R.B. and J.M.B. conducted experiments, G.H.B., J.J.G.G. and C.E.L. performed analyses and J.D. developed the ASPECT code, executed the simulations and documented the modelling effort presented in the Supplementary Information. D.J.L. contributed to the theoretical underpinnings of the kinetic theory of thermodiffusion. C.E.L. drafted the manuscript. All authors contributed to interpretations and revisions of the manuscript.
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Supplementary Information
Supplementary Discussion, Figs. 1–10 and Tables 1–3.
Supplementary Data 4
ASPECT model output for plotting.
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ASPECT model output for plotting.
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ASPECT model output for plotting.
Supplementary Data 10
ASPECT model output for plotting.
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Lesher, C.E., Dannberg, J., Barfod, G.H. et al. Iron isotope fractionation at the core–mantle boundary by thermodiffusion. Nat. Geosci. 13, 382–386 (2020). https://doi.org/10.1038/s41561-020-0560-y
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DOI: https://doi.org/10.1038/s41561-020-0560-y