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Abstract: The mobility and the rheological behaviour of magma within the Earth’s crust is controlled by magma viscosity. Crystallization and crystal morphology strongly affect viscosity, and thus mobility and eruptibility of magma, by locking it at depth or enabling its ascent towards the surface. However, the relationships between crystallinity, rheology and eruptibility remain uncertain because it is difficult to observe dynamic magma crystallization in real time. Here we show the results of in situ 3D time-dependent, high temperature, moderate pressure experiments performed under water-saturated conditions to investigate crystallization kinetics in a basaltic magma. 4D crystallization experiments with in situ view were performed using synchrotron X-ray microtomography, which provides unique quantitative information on the growth kinetics and textural evolution of pyroxene crystallization in basaltic magmas. Crystallization kinetics obtained with 4D experiments were combined with a numerical model to investigate the impact of rapid dendritic crystallization on basaltic dike propagation, and demonstrate its dramatic effect on magma mobility and eruptibility. We observe dendritic growth of pyroxene on initially euhedral cores, and a sur- prisingly rapid increase in crystal fraction and aspect ratio at undercooling ≥30 °C. Rapid dendritic crystallization favours a rheological transition from Newtonian to non-Newtonian behaviour within minutes. Modelling results show that dendritic crystallization at moderate undercooling (30-50 °C) can strongly affect magma rheology during magma ascent within a dike with important implications for the mobility of basaltic magmas within the crust. Our results provide insights into the processes that control whether magma ascent within the crust leads to eruption or not.

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Abstract: The Fe–Mg exchange coefficient between olivine (ol) and melt (m), defined as KdFe𝑇−Mg Kd Fe T − Mg  = (Feol/Fem)·(Mgm/Mgol), with all FeT expressed as Fe2+, is one of the most widely used parameters in petrology. We explore the effect of redox conditions on KdFe𝑇−Mg Kd Fe T − Mg using experimental, olivine-saturated basaltic glasses with variable H2O (≤ 7 wt%) over a wide range of fO2 (iron-wüstite buffer to air), pressure (≤ 1.7 GPa), temperature (1025–1425 °C) and melt composition. The ratio of Fe3+ to total Fe (Fe3+/∑Fe), as determined by Fe K-edge µXANES and/or Synchrotron Mössbauer Source (SMS) spectroscopy, lies in the range 0–0.84. Measured Fe3+/∑Fe is consistent (± 0.05) with published algorithms and appears insensitive to dissolved H2O. Combining our new data with published experimental data having measured glass Fe3+/∑Fe, we show that for Fo65–98 olivine in equilibrium with basaltic and basaltic andesite melts, KdFe𝑇−Mg Kd Fe T − Mg decreases linearly with Fe3+/∑Fe with a slope and intercept of 0.3135 ± 0.0011. After accounting for non-ideal mixing of forsterite and fayalite in olivine, using a symmetrical regular solution model, the slope and intercept become 0.3642 ± 0.0011. This is the value at Fo50 olivine; at higher and lower Fo the value will be reduced by an amount related to olivine non-ideality. Our approach provides a straightforward means to determine Fe3+/∑Fe in olivine-bearing experimental melts, from which fO2 can be calculated. In contrast to KdFe𝑇−Mg Kd Fe T − Mg , the Mn–Mg exchange coefficient, KdMn−Mg Kd Mn − Mg , is relatively constant over a wide range of P–T–fO2 conditions. We present an expression for KdMn−Mg Kd Mn − Mg that incorporates the effects of temperature and olivine composition using the lattice strain model. By applying our experimentally-calibrated expressions for KdFe𝑇−Mg Kd Fe T − Mg and KdMn−Mg Kd Mn − Mg to olivine-hosted melt inclusions analysed by electron microprobe it is possible to correct simultaneously for post-entrapment crystallisation (or dissolution) and calculate melt Fe3+/∑Fe to a precision of ≤ 0.04.

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Abstract: Basaltic volcanism is strongly influenced by magmatic viscosity, which, in turn, is controlled by magma composition, crystallisation, oxygen fugacity and vesiculation. We developed an environmental cell to replicate the pressure and temperature during magma ascent from crustal storage to the surface, while capturing crystallisation using in-situ 4D X-ray computed microtomography. Crystallisation experiments were performed at Diamond Light Source, using monochromatic 53 keV X-rays, a pixel size of 3.2 μm, a sample to detector distance of 2000 mm, 1440 projections per 180 deg, an acquisition time of 0.04 s, and a rotation velocity of 3.125 deg.s-1. The redox conditions were controlled using an oxidised nickel disk for each experiment. Our starting materials were samples made of crystal-free glass cylinders (Ø 3 mm) from the 2001 Etna eruption with 0.9 and 0.8 wt. % water content. In the experiments, samples and crucibles were sealed initially by applying ~10 N loads. All samples were then heated up above glass transition (between 800 °C and 900 °C) in order to allow sample homogenisation while preventing volatiles exsolution. We then pressurised each sample by applying uniaxial loads (between 80 and 380 N), using high-degree alumina pistons, in order to generate enough internal pressure to maintain bubble-free samples when the desired high temperature was reached. Once at the initial high temperature, we began experiments via dropping the temperature to different target isothermal (from 1210 to 1130 °C or 1180 to 1110 °C) and isobaric conditions (8 and 10 MPa, respectively). For the whole duration of the experiments, we were able to observe directly and record pyroxene crystal nucleation and growth. Specifically, we were able to observe pyroxene nucleation on bubbles at small undercooling (∆T) and epitaxial growth of pyroxene at large ∆T. An increase of ∆T (up to 50 °C) can be associated with a decompression of a magma chamber or a decompression during magma ascent in the conduit. As ∆T = 30 - 50 °C can be reached in most of the basaltic volcanic systems on Earth, our results provide a feasible explanation of which mechanisms control nucleation and growth of pyroxene crystals in hydrous basaltic magmas. In addition, epitaxial growth promotes a faster increase of the crystal volume. As a larger crystal content translates into a higher viscosity, our results have important implications for magma rheology, and are extremely important to improve our understanding of magma ascent dynamics during volcanic eruptions, and our capacity to predict eruptions and mitigate volcanic hazards.

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Abstract: Arc magmas erupted at the Earth's surface are commonly more oxidized than those produced at mid-ocean ridges. Possible explanations for this high oxidation state are that the transfer of fluids during the subduction process results in direct oxidation of the sub-arc mantle wedge, or that oxidation is caused by the effect of later crustal processes, including protracted fractionation and degassing of volatile-rich magmas. This study sets out to investigate the effect of disequilibrium crustal processes that may involve coupled changes in H2O content and Fe oxidation state, by examining the degassing and hydration of sulphur-free rhyolites. We show that experimentally hydrated melts record strong increases in Fe3+/∑Fe with increasing H2O concentration as a result of changes in water activity. This is relevant for the passage of H2O-undersaturated melts from the deep crust towards shallow crustal storage regions, and raises the possibility that vertical variations in fO2 might develop within arc crust. Conversely, degassing experiments produce an increase in Fe3+/∑Fe with decreasing H2O concentration. In this case the oxidation is explained by loss of H2 as well as H2O into bubbles during decompression, consistent with thermodynamic modelling, and is relevant for magmas undergoing shallow degassing en route to the surface. We discuss these results in the context of the possible controls on fO2 during the generation, storage and ascent of magmas in arc settings, in particular considering the timescales of equilibration relative to observation as this affects the quality of the petrological record of magmatic fO2.

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Abstract: A series of liquidus determinations is reported for a primitive arc basalt (15.4 wt % MgO, 45.5 wt % SiO2) from Grenada, Lesser Antilles, at anhydrous, H2O-undersaturated and H2O-saturated conditions in the pressure range 1 atm to 1.7 GPa. Fe3+/ΣFe Fe 3 + / Σ Fe of high-pressure experimental glasses as measured by μXANES ranges from 0.44 to 0.86, corresponding to oxygen fugacities (fO2) between 3.2 and 7.8 log units above the nickel–nickel oxide redox buffer (NNO). 1-atm experiments conducted from NNO − 2.5 to + 3.8 show that increasing fO2 mainly increases the forsterite content (Fo) of olivine and has little effect on phase relations. The crystallisation sequence at lower crustal pressures for all water contents is forsteritic olivine + Cr-rich spinel followed by clinopyroxene. The anhydrous liquidus is depressed by 100 and 120 °C in the presence of 2.9 and 3.8 wt % H2O, respectively. H2O-undersaturated experiments at NNO + 3.2 to + 4.5 produce olivine of equivalent composition to the most primitive olivine phenocrysts in Grenadan picrites (Fo91.4). We conclude that direct mantle melts originating beneath Grenada could be as oxidised as ~NNO + 3, consistent with the uppermost estimates from olivine–spinel oxybarometry of high Mg basalts. μXANES analyses of olivine-bearing experimental glasses are used to develop a semi-empirical oxybarometer based on the value of 𝐾𝐷Fe−Mgol−melt K D o l − m e l t F e − M g when all Fe is assumed to be in the Fe2+ state (𝐾Fe𝑇𝐷 K D F e T ). The oxybarometer is tested on an independent data set and is able to reproduce experimental fO2 to ≤1.2 log units. Experiments also show that the geochemically and petrographically distinct M- and C-series lavas on the island can be produced from hydrous melting of a common picritic source. Low pressures expand the olivine stability field at the expense of clinopyroxene, enriching an evolving melt in CaO and forcing differentiation to take place along a C-series liquid line of descent. Higher pressure conditions allow early and abundant clinopyroxene crystallisation, rapidly depleting the melt in both CaO and MgO, and thus creating the M-series.