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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: Crystallisation is a complex process that significantly affects the rheology of magma, and thus the flow dynamics during a volcanic eruption. For example, the evolution of crystal fraction, size and shape has a strong impact on the surface crust formation of a lava flow, and accessing such information is essential for accurate modelling of lava flow dynamics. To investigate the role of crystallisation kinetics on lava flow behaviour, we performed real-time, in situ synchrotron X-ray microtomography, studying the influence of temperature-time paths on the nucleation and growth of clinopyroxene and plagioclase in an oxidised, nominally anhydrous basaltic magma. Crystallisation experiments were performed at atmospheric pressure in air and temperatures from 1250 °C to 1100 °C, using a bespoke high-temperature resistance furnace. Depending on the cooling regime (single step versus continuous), two different crystal phases (either clinopyroxene or plagioclase) were produced, and we quantified their growth from both global and individual 3D texture analyses. The textural evolution of charges suggests that suppression of crystal nucleation is due to changes in the melt composition with increasing undercooling and time. Using existing viscosity models, we inferred the effect of crystals on the viscosity evolution of our crystal-bearing samples to trace changes in rheological behaviour during lava emplacement. We observe that under continuous cooling, both the onsets of the pāhoehoe-‘a‘ā transition and of non-Newtonian behaviour occur within a shorter time frame. With varying both temperature and time, we also either reproduced or approached the clinopyroxene and plagioclase phenocryst abundances and compositions of the Etna lava used as starting material, demonstrating that real-time synchrotron X-ray tomography is an ideal approach to unravel the final solidification history of basaltic lavas. This imaging technology has indeed the potential to provide input into lava flow models and hence our ability to forecast volcanic hazards.

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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: Magma crystallisation is a fundamental process driving eruptions and controlling the style of volcanic activity. Crystal nucleation delay, heterogeneous and homogeneous nucleation and crystal growth are all time-dependent processes, however, there is a paucity of real-time experimental data on crystal nucleation and growth kinetics, particularly at the beginning of crystallisation when conditions are far from equilibrium. Here, we reveal the first in situ 3D time-dependent observations of crystal nucleation and growth kinetics in a natural magma, reproducing the crystallisation occurring in real-time during a lava flow, by combining a bespoke high-temperature environmental cell with fast synchrotron X-ray microtomography. We find that both crystal nucleation and growth occur in pulses, with the first crystallisation wave producing a relatively low volume fraction of crystals and hence negligible influence on magma viscosity. This result explains why some lava flows cover kilometres in a few hours from eruption inception, highlighting the hazard posed by fast-moving lava flows. We use our observations to quantify disequilibrium crystallisation in basaltic magmas using an empirical model. Our results demonstrate the potential of in situ 3D time-dependent experiments and have fundamental implications for the rheological evolution of basaltic lava flows, aiding flow modelling, eruption forecasting and hazard management.