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The Skaergaard intrusion is one of the most thoroughly studied layered mafic intrusions on Earth and an exceptional example of (near) closed-system magmatic differentiation. We report new Fe isotope data for whole rocks, and magnetite and ilmenite separates through the layered series (LS) and upper border series (UBS) of the intrusion. δ56Fe values for gabbroic rocks range from 0.033‰ to 0.151‰ with an abrupt step increase at the base of Lower Zone c (LZc) within LS with the appearance of cumulus magnetite and subsequent decline accompanying FeTi oxide fractionation. The lowest δ56Fe values are found near the Upper Zone b (UZb) to c (UZc) boundary followed by a sharp rise across UZc approaching the Sandwich Horizon. Magnetite–ilmenite separates straddle bulk rock compositions with fractionation factors (Δ56Femt-ilm) of 0.081‰ to 0.239‰, consistent with subsolidus equilibration. Granophyric rocks occurring as pods, sheets and wispy layers from the upper zone and UBS equivalents and having unradiogenic Sr similar to gabbroic rocks of Skaergaard, are isotopically heavier than their host ferrodiorites (Δ56Fegranophyre-ferrodiorite ≥ 0.1‰) reaching a maximum δ56Fe of 0.217‰ in UBS. A fused xenolith from UBS has δ56Fe = 0.372‰. This range in δ56Fe spans much of that reported for terrestrial igneous rocks, and like the global dataset, shows a pronounced increase in δ56Fe with inferred silica content of modeled Skaergaard liquids.

Forward modeling of closed system fractional solidification was undertaken to account for Fe isotope systematics, first by testing published liquid lines of descent (LLD), and then by exploring improvements and considering the impacts of liquid immiscibility, crustal contamination, fluid exsolution and diffusional processes. Our modeling relies on published Fe+2 and Fe+3 force constants for magmatic minerals and silicate glasses, and the most reliable estimates of the average bulk composition and mass proportions of the well-defined subzones of the intrusion. We show that the increase in δ56Fe across the LZb–LZc boundary is readily explained by the increased incorporation of Fe+3 into the crystallizing solid including magnetite. We further demonstrate that the classic Fenner LLD, involving strong Fe enrichment at nearly constant silica, does not lead to a rise in δ56Fe toward the end stages of evolution, while a Bowen-like LLD, with little Fe enrichment and strong Si enrichment, also underestimates enrichment in heavy Fe isotopes in the ferrodiorites of UZc. A LLD following an intermediate path involving modest Fe and Si enrichment, followed by Fe depletion best explains the observations. We predict ~3.5% (by mass) residual liquid after crystallization of UZc having a composition similar to felsic segregations in pegmatitic bodies found in the intrusion. While liquid immiscibility may have been encountered within fractionating mush at the margins of the intrusion, the Fe isotope systematics do not support liquid phase separation of the bulk magma. Crustal contamination, fluid exsolution, hydrothermal alteration and thermal diffusion are also shown to have no resolvable effect on the Fe isotope composition of the gabbroic and granophyric rocks. We conclude that the Fe isotope systematics documented in the Skaergaard intrusion reflect the dominant role of fractionating Fe-rich minerals from gabbroic through ferrodioritic to rhyolitic liquids. The success of our model to account for the observed Fe isotope systematics for Skaergaard demonstrates the utility of Fe+2 and Fe+3 force constants determined at ambient conditions to model magmatic conditions and gives critical insights into plutonic processes fractionating Fe isotopes complementary to the volcanic record.

 

SUMMARY Anisotropy of remanent magnetization and magnetic susceptibility are highly sensitive and important indicators of geological processes which are largely controlled by mineralogical parameters of the ferrimagnetic fraction in rocks. To provide new physical insight into the complex interaction between magnetization structure, shape, and crystallographic relations, we here analyse ‘slice-and-view’ focused-ion-beam (FIB) nano-tomography data with micromagnetic modelling and single crystal hysteresis measurements. The data sets consist of 68 magnetite inclusions in orthopyroxene (Mg60) and 234 magnetite inclusions in plagioclase (An63) were obtained on mineral separates from the Rustenburg Layered Suite of the Bushveld Intrusive Complex, South Africa. Electron backscatter diffraction was used to determine the orientation of the magnetite inclusions relative to the crystallographic directions of their silicate hosts. Hysteresis loops were calculated using the finite-element micromagnetics code MERRILL for each particle in 20 equidistributed field directions and compared with corresponding hysteresis loops measured using a vibrating sample magnetometer (VSM) on silicate mineral separates from the same samples. In plagioclase the ratio of remanent magnetization to saturation magnetization (Mrs/Ms) for both model and measurement agree within 1.0 per cent, whereas the coercivity (Hc) of the average modelled curve is 20 mT lower than the measured value of 60 mT indicating the presence of additional sources of high coercivity in the bulk sample. The VSM hysteresis measurements of the orthopyroxene were dominated by multidomain (MD) magnetite, whereas the FIB location was chosen to avoid MD particles and thus contains only particles with diameters <500 nm that are considered to be the most important carriers of palaeomagnetic remanence. To correct for this sampling bias, measured MD hysteresis loops from synthetic and natural magnetites were combined with the average hysteresis loop from the MERRILL models of the FIB region. The result shows that while the modelled small-particle fraction only explains 6 per cent of the best fit to the measured VSM hysteresis loop, it contributes 28 per cent of the remanent magnetization. The modelled direction of maximal Mrs/Ms in plagioclase is subparallel to [001]plag, whereas Hc does not show a strong orientation dependence. The easy axis of magnetic remanence is in the direction of the magnetite population normal to (150)plag and the maximum calculated susceptibility (χ*) is parallel to [010]plag. For orthopyroxene, the maximum Mrs/Ms, maximum χ* and the easy axis of remanence is strongly correlated to the elongation axes of magnetite in the [001]opx direction. The maximum Hc is oriented along [100]opx and parallel to the minimum χ*, which reflects larger vortex nucleation fields when the applied field direction approaches the short axis. The maximum Hc is therefore orthogonal to the maximum Mrs/Ms, controlled by axis-aligned metastable single-domain states at zero field. The results emphasize that the nature of anisotropy in natural magnetite does not just depend on the particle orientations, but on the presence of different stable and metastable domain states, and the mechanism of magnetic switching between them. Magnetic modelling of natural magnetic particles is therefore a vital method to extract and process anisotropic hysteresis parameters directly from the primary remanence carriers.