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1. Identifying the granitic composition water-saturated solidus

   Rufledt C, Thomas JB (September 2023, Xth Hutton Symposium)

   The granitic water-saturated solidus (G-WSS) is the lower temperature limit of magmatic mineral crystallization. The accepted water-saturated solidus for granitic compositions was largely determined >60 years ago1. More recent advances in experimental petrology, improved analytical techniques, and recent observations that granitic systems can remain active or spend a significant proportion of their lives at conditions below the traditional G-WSS2–5 necessitate a careful experimental investigation of the near-solidus regions of granitic systems. Natural and synthetic starting materials were melted at 10 kbar and 900°C with 48 wt% H2O to produce hydrous glasses for subsequent experiments at lower PT conditions used to locate the G-WSS. We performed crystallization experiments and melting experiments at temperatures ranging from 575 to 800°C and 1, 6, 8, and 10 kbar on 12 granitoid compositions. First, we ran a series of isothermal crystallization experiments along each isobar at progressively lower temperatures until runs completely crystallized to identify apparent solidus temperatures. Geochemical analyses of quenched glass compositions demonstrate that progressive crystallization drives all starting compositions towards silica-rich, water-saturated rhyolitic/granitic melts (e.g., ~7578 wt% SiO2). After identifying the apparent solidus temperatures at which the various compositions crystallized, we then ran series of reversal-type melting experiments. With the goal of producing rocks with hydrous equilibrium microstructures, we crystallized compositions at temperatures ~10°C below the apparent solidus identified in crystallization experiments, and then heated isobarically to conditions that produced ~20% melt during the crystallization experiments. Importantly, crystallization experiments and heating experiments at the same PT conditions produced similar proportions of melt, crystals, and vapor. A time-series of experiments 230 days at PT conditions previously identified to produce ~10% to 20% melt did not reveal any kinetic effects on melt crystallization. Experiments at 6 to 10 kbar crystallized/melted at temperatures close to the published G-WSS. However, at lower pressures where the published G-WSS is strongly curved in PT space, all compositions investigated contained melt to temperatures ~75 to 100°C below the accepted G-WSS. The similarity of crystallization temperatures for the higher-pressure experiments to previously published results, similar phase proportions in melting and crystallization experiments, and the lack of kinetic effects on crystallization collectively suggest that our lower pressure constraints on the G-WSS are accurate. The new experimental results demonstrating that the lower-pressure G-WSS is significantly lower than unanimously accepted estimates will help us to better understand the storage conditions, evolution, and potential for eruption in mid- to upper-crustal silicic magmatic systems. (1) Tuttle, O.; Bowen, N. Origin of Granite in the Light of Experimental Studies in the System NaAlSi3O8–KAlSi3O8–SiO2–H2O; Geological Society of America Memoirs; Geological Society of America, 1958; Vol. 74. https://doi.org/10.1130/MEM74. (2) Rubin, A. E.; Cooper, K. M.; Till, C. B.; Kent, A. J. R.; Costa, F.; Bose, M.; Gravley, D.; Deering, C.; Cole, J. Rapid Cooling and Cold Storage in a Silicic Magma Reservoir Recorded in Individual Crystals. Science 2017, 356 (6343), 1154–1156. https://doi.org/10.1126/science.aam8720. (3) Andersen, N. L.; Jicha, B. R.; Singer, B. S.; Hildreth, W. Incremental Heating of Bishop Tuff Sanidine Reveals Preeruptive Radiogenic Ar and Rapid Remobilization from Cold Storage. Proceedings of the National Academy of Sciences 2017, 114 (47), 12407–12412. https://doi.org/10.1073/pnas.1709581114. (4) Ackerson, M. R.; Mysen, B. O.; Tailby, N. D.; Watson, E. B. Low-Temperature Crystallization of Granites and the Implications for Crustal Magmatism. Nature 2018, 559 (7712), 94–97. https://doi.org/10.1038/s41586-018-0264-2. (5) Glazner, A. F.; Bartley, J. M.; Coleman, D. S.; Lindgren, K. Aplite Diking and Infiltration: A Differentiation Mechanism Restricted to Plutonic Rocks. Contributions to Mineralogy and Petrology 2020, 175 (4). https://doi.org/10.1007/s00410-020-01677-1. 

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2. Insights on Arc Magmatic Systems Drawn from Natural Melt Inclusions and Crystallization Experiments at P H2O   = 800 MPa under Oxidizing Conditions

   https://doi.org/10.1093/petrology/egae117  

   Andrys, Janine L; Cottrell, Elizabeth; Kelley, Katherine A; Waters, Laura E; Coombs, Michelle L (December 2024, Journal of Petrology)

   Abstract Whole rock compositions at Buldir Volcano, western Aleutian arc, record a strong, continuous trend of iron depletion with decreasing MgO, classically interpreted as a calc-alkaline liquid line of descent. In contrast, olivine-hosted melt inclusions have higher total iron (FeO*) than whole rocks and show little change in FeO* with decreasing MgO. To investigate this discrepancy and determine the conditions required for strong iron depletion, we conducted oxygen fugacity (ƒO2) buffered, water-saturated crystallization experiments at 800 MPa and ƒO2 = QFM + 1.6 ± 0.4 (1$$\sigma$$) (where QFM refers to the quartz-fayalite-magnetite buffer) on a high-Al, basaltic starting material modeled after a Buldir lava. Experimental conditions were informed by olivine-hosted melt inclusions that record minimum entrapment pressures as high as 570 MPa, >6 wt % H2O, and ƒO2 of QFM + 1.4 (±0.2), making Buldir one of the most oxidized and wettest arc volcanoes documented globally. The experiments produce melts with Si-enrichment and Fe-depletion signatures characteristic of evolved, calc-alkaline magmas at the lowest MgO, although FeO* remains roughly constant over most of the experimental temperature range. Experiments saturate CrAl-spinel and olivine at 1160°C, followed by clinopyroxene and Al-spinel at 1085°C, hornblende at 1060°C, and, finally, plagioclase and magnetite between 1040°C and 960°C. Hornblende crystallization, not magnetite, generates the largest increase in SiO2 and largest decrease in FeO* in coexisting melts. Compositions of melt inclusions are consistent with experimental melts and reflect crystallization of a basaltic parent magma at high PH2O. In contrast, the whole rock compositional trends are influenced by magma mixing and phenocryst redistribution and accumulation. The crystallization experiments and natural liquids (melt inclusions and groundmass glass) from Buldir suggest that for an oxidized, hydrous primary basalt starting composition, significant Fe depletion from the melt will not occur until intermediate to late stages of magma crystallization (< ~4.5 wt % MgO). We conclude that the Buldir whole rock trend cannot be reproduced by crystallization at arc-relevant oxygen fugacities and is not a true liquid line of descent, warranting caution when interpreting volcanic trends globally. 

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3. Experimentally derived F, Cl, and Br fluid/melt partitioning of intermediate to silicic melts in shallow magmatic systems

   https://doi.org/10.2138/am-2022-8109  

   Cassidy, Mike; Iveson, Alexander A; Humphreys, Madeleine CS; Mather, Tamsin A; Helo, Christoph; Castro, Jonathan M; Ruprecht, Philipp; Pyle, David M (October 2022, American Mineralogist)

   Abstract The conditions under which halogens partition in favor of an exsolved fluid relative to the coexisting melt are key for understanding many magmatic processes, including volcanic degassing, evolution of crustal melt bodies, and ore formation. We report new F, Cl, and Br fluid/melt partition coefficients for intermediate to silicic melts, for which F and Br data are particularly lacking; and for varying CO2-H2O contents to assess the effects of changing fluid composition (XH2O) on Br fluid/melt partitioning for the first time. The experiments were conducted at pressures 50–120 MPa, temperatures 800–1100 °C, and volatile compositions [molar XH2O = H2O/(H2O +CO2)] of 0.55 to 1, with redox conditions around the Nickel-Nickel Oxygen buffer (fO2 ≈ NNO). Experiments were not doped with Cl, Br, or F and were conducted on natural crystal-bearing volcanic products at conditions close to their respective pre-eruptive state. The experiments therefore provide realistic constraints on halogen partitioning at naturally occurring, brine-undersaturated conditions. Measurements of Br, Cl, and F were made by Secondary Ion Mass Spectrometry (SIMS) on 13 experimental glass products spanning andesite to rhyolitic compositions, together with their natural starting materials from Kelud volcano, Indonesia, and Quizapu volcano, Chile. Fluid compositions were constrained by mass balance. Average bulk halogen fluid/melt partition coefficients and standard deviations are: DClfluid/melt = 3.4 (±3.7 1 s.d.), DFfluid/melt = 1.7 (±1.7), and DBrfluid/melt = 7.1 (±6.4) for the Kelud starting material (bulk basaltic andesite), and DClfluid/melt = 11.1 (±3.5), DFfluid/melt = 0.8 (±0.8), and DBrfluid/melt = 31.3 (±20.9) for Quizapu starting material (bulk dacite). The large range in average partition coefficients is a product of changing XH2O, pressure and temperature. In agreement with studies on synthetic melts, our data show an exponential increase of halogen Dfluid/melt with increasing ionic radius, with partitioning behavior controlled by melt composition according to the nature of the complexes forming in the melt (e.g., SiF4, NaCl, KBr). The fundamental chemistry of the different halogens (differing ionic size and electronegativities) controls the way in which partitioning responds to changes in melt composition and other variables. Experimental results confirm that more Cl partitions into the fluid at higher bulk Cl contents, higher melt Na, higher fluid XH2O ratios, and lower temperatures. Bromine shows similar behavior, though it seems to be more sensitive to temperature and less sensitive to Na content and XH2O. In contrast, F partitioning into the fluid increases as the melt silica content decreases (from 72 to 56 wt% SiO2), which we attribute to the lower abundance of Si available to form F complexes in the melt. These new data provide more insights into the conditions and processes that control halogen degassing from magmas and may help to inform the collection and interpretation of melt inclusions and volcano gas data. 

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4. Barometers Behaving Badly II: a Critical Evaluation of Cpx-Only and Cpx-Liq Thermobarometry in Variably-Hydrous Arc Magmas

   https://doi.org/10.1093/petrology/egad050  

   Wieser, Penny E; Kent, Adam_J R; Till, Christy B (August 2023, Journal of Petrology)

   The chemistry of erupted clinopyroxene crystals (±equilibrium liquids) have been widely used to deduce the pressures and temperatures of magma storage in volcanic arcs. However, the large number of different equations parameterizing the relationship between mineral and melt compositions and intensive variables such as pressure and temperature yield vastly different results, with implications for our interpretation of magma storage conditions. We use a new test dataset composed of the average Clinopyroxene-Liquid (Cpx-Liq) compositions from N = 543 variably hydrous experiments at crustal conditions (1 bar to 17 kbar) to assess the performance of different thermobarometers and identify the most accurate and precise expressions for application to subduction zone magmas. First, we assess different equilibrium tests, finding that comparing the measured and predicted Enstatite-Ferrosillite and KD (using Fet in both phases) are the most useful tests in arc magmas, whereas CaTs, CaTi and Jd tests have limited utility. We then apply further quality filters based on cation sums (3.95–4.05), number of analyses (N > 5) and the presence of reported H2O data in the quenched experimental glass (hereafter ‘liquid’) to obtain a filtered dataset (N = 214). We use this filtered dataset to compare calculated versus experimental pressures and temperatures for different combinations of thermobarometers. A number of Cpx-Liq thermometers perform very well when liquid H2O contents are known, although the Cpx composition contributes little to the calculated temperature relative to the liquid composition. Most Cpx-only thermometers perform very badly, greatly overestimating temperatures for hydrous experiments. These two findings demonstrate that the Cpx chemistry alone holds very little temperature information in hydrous systems. Most Cpx-Liq and Cpx-only barometers show similar performance to one another (mostly yielding root mean square errors [RMSEs] of 2–3.5 kbar), although the best Cpx-only barometers currently outperform the best Cpx-Liq barometers. We also assess the sensitivity of different equations to melt H2O contents, which are poorly constrained in many natural systems. Overall, this work demonstrates that Cpx-based barometry on individual Cpx only provides sufficient resolution to distinguish broad storage regions in continental arcs (e.g. upper, mid, lower crust). Significant averaging of Cpx compositions from experiments reported at similar pressures can reduce RMSEs to ~1.3–1.9 kbar. We hope our findings motivate the substantial amount of experimental and analytical work that is required to obtain precise and accurate estimates of magma storage depths from Cpx ± Liq equilibrium in volcanic arcs. 

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5. Evidence of Rapid Phenocryst Growth of Olivine During Ascent in Basalts From the Big Pine Volcanic Field: Application of Olivine‐Melt Thermometry and Hygrometry at the Liquidus

   https://doi.org/10.1029/2020GC009264  

   Brehm, Sarah K.; Lange, Rebecca A. (October 2020, Geochemistry, Geophysics, Geosystems)

   Abstract The Quaternary Big Pine (BP) volcanic field in eastern California is notable for the occurrence of mantle xenoliths in several flows. This points to rapid ascent of basalt through the crust and precludes prolonged storage in a crustal reservoir. In this study, the hypothesis of phenocryst growth during ascent is tested for several basalts (13–7 wt% MgO) and shown to be viable. Phenocrysts of olivine and clinopyroxene frequently display diffusion‐limited growth textures, and clinopyroxene compositions are consistent with polybaric crystallization. When the most Mg‐rich olivine in each sample is paired with the whole‐rock composition, resulting(olivine‐melt) values (0.31–0.36) match those calculated from literature models (0.32–0.36). Application of a Mg‐ and a Ni‐based olivine‐melt thermometer from the literature, both calibrated on the same experimental data set, leads to two sets of temperatures that vary linearly with whole‐rock MgO wt%. Because the Ni thermometer is independent of water content, it provides the actual temperature at the onset of olivine crystallization (1247–1097°C), whereas the Mg thermometer gives the temperature under anhydrous conditions and thus allows ΔT(=T_Mg − T_Ni = depression of liquidus due to water) to be obtained. The average ΔTfor all samples is ~59°C, which is consistent with analyzed water contents of 1.5–3.0 wt% in olivine‐hosted melt inclusions from the literature. Because the application of olivine‐melt thermometry/hygrometry at the liquidus only requires microprobe analyses of olivine combined with whole‐rock compositions, it can be used to obtain large global data sets of the temperature and water contents of basalts from different tectonic settings. 

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