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The origin of clinopyroxene-titanomagnetite clustering during crystallisation of synthetic trachybasalt
No full textCrystal clustering impacts rheology and differentiation in magmatic systems, and also offers insights into nucleation processes. Electron backscatter diffraction (EBSD) is ideal for studying interactions between crystals at interfaces. Clinopyroxene (Cpx) – titanomagnetite (Timt) clusters formed in time series experiments on synthetic trachybasaltic melt were studied using EBSD to understand the cause of clustering. Experiments were performed at 400 MPa and the NNO +2 buffer, at both anhydrous and hydrous (2 wt.% H2O) conditions, by cooling from 1300 °C (superliquidus) to 1100 °C with a rate of 80°C/min and holding at the target temperature for 4 – 8 hours before isobaric quenching.
All experiments crystallize dendritic Cpx (Lmax = 50 – 60 μm) and isometric euhedral to hopper-shaped Timt (Lmax = 5 – 6 μm). Infrequent (~ 10 mm-2) unmelted Cr-oxide crystals are surrounded by polycrystalline Cr-bearing Timt rims (Lmax Cr-oxide + rim = 20 μm). Cpx dendrite “rosettes” radiate from the polycrystalline rims, but many dendrites do not belong to rosettes, at least in 2D. Individual Timt crystals (Cr-free) are strongly associated with the sides and tips of Cpx dendrites. About 75% of Timt grains are in contact with Cpx in 2D. Cpx-Timt interfaces are irregular, and Timt is often attached only by thin necks. Timt grain centers are weakly clustered (R = 0.87 – 0.95, 1 = random).
Timt shows a strong crystallographic orientation relationship (COR) with Cpx, with 75 – 89% of Timt grains in contact with Cpx lying within 6° of a single fixed (“specific”) COR, OR1 = Cpx [010] // Timt <110>; Cpx (100) // Timt <111>; Cpx [001] // Timt <112>. The axes Cpx [010] // Timt <110> show the least dispersion (< 3°) from the ideal alignment. Relative to Cpx, individual Timt may be rotated up to 6° away from OR1, around an axis close to Cpx [010]. There are two peaks in this continuous distribution, corresponding to OR1 (above) and OR2 = Cpx [010] // Timt <110>; Cpx (-101) // Timt <111>; Cpx [101] // Timt <112>. The misorientation between OR1 and OR2 is 5.3°. OR1 and OR2 together represent 68 – 77% of Timt grains in contact with Cpx (tolerance angle 2.6°).
Cpx dendrite branches bend around Cpx [010]. The anhydrous sample with dwell time 4 hours shows continuous bending of up to ~15°, whereas the hydrous sample with dwell time 8 hours shows bending of up to only ~7° and subgrain boundaries (1 - 2°) separating undistorted domains, suggesting recovery of bent crystals during annealing. Initial Cpx nucleation likely occurred heterogeneously as rosettes on Cr-bearing Timt rims around Cr-oxide crystals. Multiple Timt grains touching different branches of the same bent Cpx crystal all maintain a close COR with the Cpx orientation immediately adjacent to the Cpx-Timt interface, indicating that Timt nucleated on (or attached to) dendrite branches during or after their growth.
In conclusion, EBSD is a powerful method for understanding crystallization and cluster formation. Future work will study the effect of annealing time, water content, and undercooling on Cpx – Timt cluster development
Crystallization kinetics of clinopyroxene and titanomagnetite growing from a trachybasaltic melt: New insights from isothermal time-series experiments
No full textThe effect of melt water content and isothermal annealing time on the formation and evolution of clinopyroxene-titanomagnetite clusters
No full textCrystal clustering influences the formation of crystal mushes and the rheology and differentiation of magmas. Heterogeneous nucleation is known to be an important cluster-forming mechanism, but there has been little systematic experimental study of cluster formation and evolution.In this study, we analysed dynamic crystallization experiments from Pontesilli et al. (2019), focusing on clusters of clinopyroxene (cpx) and titanomagnetite (tmt). These experiments aimed to reproduce the crystallisation behaviour of dry (nominally 0 wt.% H2O) and hydrous (2 wt.% H2O added) Etnean trachybasalt at mid-crustal storage conditions (400 MPa, 1100°C, NNO+1 oxygen buffer, corresponding to undercooling of 120°C and 80°C respectively). After superheating at 1300°C for 30 minutes, samples were cooled at 80°C/min to 1100°C and annealed for dwell times ranging from 0.5h to 8h.Electron backscatter diffraction (EBSD) maps and image analysis were used to quantify clustering parameters such as tmt number density, "shared perimeter fraction" ("SPF", the fraction of total tmt boundary length shared between cpx and tmt), "fraction of touching tmt" ("FTT", the fraction of all tmt grains that are touching cpx), and the crystallographic orientation relationships (CORs) between cpx and tmt. Dry samples generally show a higher number density of tmt crystals than wet samples. SPF and FTT are highest (≥ 0.40 and ≥ 0.93 respectively) in the 0.5h duration dry experiments. Both parameters fall to ≤ 0.25 and ≤ 0.75 respectively after 4h of annealing. In wet experiments, SPF and FFT are lower (≤ 0.33 and ≤ 0.79 respectively) at 0.5h annealing time and do not decrease strongly with annealing.EBSD maps reveal that > 70 % of tmt grains are in contact with cpx in all analysed samples. Tmt exhibits two closely related CORs to cpx. More than 60% of total tmt-cpx boundary length in all samples follows COR 1 ([-110]tmt[010]cpx, [111]tmt(100)*cpx, [-1-12]tmt[001]cpx) or COR 2 ([-110]tmt[010]cpx, [-1-11]tmt(-101)*cpx, [112]tmt[101]cpx). COR frequencies suggest a strong influence of water content and annealing time on their formation. In the 0.5h duration dry experiment, tmt-cpx boundaries following COR 1 are twice as frequent by length as those following COR 2, whereas in the 0.5h duration wet experiment, COR 2 boundaries are 5 times more frequent by length than COR 1 boundaries. In both wet and dry experiments the length ratio of COR 1 : COR 2 boundaries approaches 1 with longer annealing times.The degree of undercooling (as imposed by the different water contents) is the most important influence on the microstructural clustering parameters, leading to lower overall number densities of tmt as well as affecting the SPF and FTT values at short durations and the subsequent evolution of these parameters with increasing annealing time. The high frequency of tmt-cpx CORs is consistent with heterogeneous nucleation. However, the mechanisms controlling which CORs develop are unclear. Annealing does not fully erase CORs or microstructural signatures of clustering, suggesting that crystal clusters erupted in volcanic products could still preserve signs of their formation
Re-equilibration of clinopyroxene-titanomagnetite clusters: the effect of isothermal annealing time and melt water content
No full textExperimental observation of extremely rapid clinopyroxene growth in a trachybasaltic melt: Clues on phenocryst crystallization kinetics in naturally cooled magmas
No full textTitanomagnetite-clinopyroxene clustering in synthetic trachybasalts: Insight into nucleation mechanisms from new experimental samples
No full textThermodynamics and kinetics of cation partitioning between plagioclase and trachybasaltic melt in static and dynamic systems: A reassessment of the lattice strain and electrostatic energies of substitution
No full textMost of the solidification history of magmas beneath active volcanoes takes place in chemically and physically perturbed plumbing systems where the growth of crystals is collectively governed by a range of kinetic processes related to the dynamics of crustal reservoirs and eruptive conduits. In this context, we have experimentally investigated the partitioning of major, minor, and trace cations between plagioclase and trachybasaltic melt under conventional static (no physical perturbation) and dynamic (melt stirring) crystallization regimes. Slow interface reaction kinetics are established between the advancing crystal surface and the adjacent melt, as the result of the combined control of a small degree of effective undercooling, prolonged diffusive relaxation, and convective homogenization. The kinetic aspects of plagioclase growth influence the partitioning of trace cations during transport of structural units across the crystal-melt interface, with consequent departure from macroscopic equilibrium in the system. The type and number of charge-balanced and -imbalanced configurations produced by the accommodation of trace cations into the coordination polyhedron can be thermodynamically rationalized in terms of lattice strain and electrostatic partitioning energetics. However, the overall solution energy accompanying trace cation kinetic substitutions cannot be entirely deconvoluted from major component activities in both melt and plagioclase phases. The emerging view that slow interface kinetic processes may lead to strong compositional dependence for the partition coefficient in dynamic subvolcanic environments contrasts markedly with the conventional idea that the energetics of cation partitioning are dominantly controlled by the effect of isothermal changes in the bulk system
Crystallization kinetics of clinopyroxene and titanomagnetite growing from a trachybasaltic melt: New insights from isothermal time-series experiments
Full text linkIn order to investigate the role of crystallization kinetics in mafic alkaline systems, textural measurements, mineral compositional changes and diffusion modelling calculations have been carried out on isothermal time-series experiments. The data were obtained at 400 MPa and 1100 °C under anhydrous (nominally 0 wt% H 2 O) and hydrous (2 wt% H 2 O added) conditions. A synthetic trachybasaltic melt was first heated up to the superliquidus temperature of 1300 °C and then rapidly cooled at 80 °C/min down to 1100 °C. The final target temperature was kept constant over variable dwell times in the range of 0.5–24 h. Results from textural analysis indicate the attainment of fast crystal growth kinetics at the shortest experimental run duration, with early achievement of stable crystal sizes for clinopyroxene and titanomagnetite. The surface area to volume ratio weakly decreases with increasing dwell time, according to the development of euhedral crystal morphologies. Crystal growth rates are also observed to progressively decrease from 0.5 to 24 h. Due to the effect of fast growth kinetics, the morphological maturation of clinopyroxene progresses by attachment of dendrite branches, infilling and overgrowth phenomena, leading to the formation of well-faced and euhedral crystals. The kinetically-controlled cation exchange (Si + Mg) → ( T Al + Fe 3+ ) controls the clinopyroxene compositional variation, expanding the stability of Tschermak component at the expense of diopside. Conversely, titanomagnetite is characterized by an almost constant composition that, however, is enriched in incompatible Al and Mg cations, as typically observed under rapid crystal growth conditions. Titanomagnetite crystals show always euhedral morphology that develops by heterogeneous nucleation on early-formed clinopyroxene dendrites. Overall, the effect of undercooling causes strong supersaturation phenomena in the trachybasaltic melt, resulting in enhanced nucleation kinetics and fast attainment of a high crystallinity. As the dwell time increases, the bulk system tends to minimize the interfacial free energy between crystals and surrounding melt. This results in the progressive replacement of the early dendritic shapes developed in a diffusion-limited growth regime, by the formation of euhedral morphologies typical of interface-limited regimes that still retain the chemical evidences of the dendritic stage as complex zoning patterns in clinopyroxene
Magma titanium and iron contents dictate crystallization timescales and rheological behaviour in basaltic volcanic systems
Full text linkMagma ascending through Earth’s crust undergoes complex chemical and physical changes that may
induce crystallization, a process that contributes to lead the magmatic system toward a
thermodynamic state of equilibrium. The diverse cooling and deformative regimes suffered by
magmas heavily influence crystallization rates, solidification timescales, and consequently, the
rheological evolution of magma. This, in turn, significantly impacts the dynamics of volcanic plumbing
systems and the associated eruptive styles. Here, we investigate the rheological changes in Stromboli
magma (Italy) during disequilibrium crystallization under non-isothermal subliquidus conditions. By
systematically varying the cooling rate (1-10 °C/min) and the shear rate (1-10 s−1), we find that cooling
rates significantly influence the solidification path of the basalt, whereas shear rates have a
subordinate effect. By comparing our results with literature data on basalts from Mt. Etna
(Italy), characterized by higher TiO2 and FeOtot contents, we observed distinct timescales
and rates of solidification, contributing to unique eruptive dynamics in these volcanic plumbing
systems
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