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In basaltic volcanic ash recovered from a seamount at 3000 m water depth, we discovered marcasite and pyrite precipitation within cavities that formed by partial to complete dissolution of olivine. In places, these cavities are reminiscent of negative crystal shapes; elsewhere they apparently continue along cracks. In strong contrast, adjacent volcanic glass shows little, if any, evidence for dissolution. The FeS2 precipitates were commonly found to be conjoined and planar aggregates, occurring in the center of the voids. Their maximum volume fraction in relation to the void space as determined by 2D and 3D imaging techniques corresponds to the amount of iron released by olivine dissolution. Almost all occurrences of FeS2 precipitation are related to Cr-spinel inclusions in the former olivine. We propose that rapid olivine dissolution was initiated by reduced H2S-bearing fluids at olivine grain boundaries or surfaces exposed by cracks. Many of these cracks are connected to spinel grains, where the iron liberated from olivine is mineralized as FeS2, initially facilitated by heterogeneous nucleation. Subsequent pyrite and/or marcasite precipitation occurred as overgrowths on existing FeS2 aggregates. The particular chemical environment of low-pH, hydrogen sulfide-bearing fluids may have enhanced olivine dissolution by (1) keeping Fe in solution and (2) sequestering important quantities of Fe as FeS2. The in situ oxidation of ferrous Fe and precipitation of ferric hydroxides at the olivine surface commonly observed in oxic environments were obviously impeded. It would have slowed down olivine dissolution to rates more similar to the dissolution of basaltic glass. We have no direct indication that the process of rapid olivine dissolution was aided by subseafloor life. However, the presence of fibrous structures with small sulfide particles could indicate late colonization of sulfate-reducing bacteria that may add an additional path of iron fixation.

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Magma-sediment mingling occurring in shallow porous sediments is mainly investigated through field observations of old exhumed rift basins. During the IODP Expedition 385 we have drilled through the shallow sills emplaced in the active rift of the Guaymas Basin, Gulf of California. The results of this expedition enable a pioneer study of the impact of recent magma-sediment mingling processes leading to peperite formation. Furthermore, it provides a present-day geological context to investigate and quantify the impact of this mingling process on the element cycles in subsurface sediments, and temporal evolution of the microbial habitat associated with epithermal hydrothermal fluid circulation. Our approach of exploring magma-sediment mingling processes includes laboratory experiments, numerical modelling, and identification of specific field analogues in addition to petrological and geochemical constraints.Using these modern techniques, we review here the discoveries made during the IODP Expedition 385 and present preliminary results from our post-cruise research from the perspective of the peperite formation. We report here petrographic and geochemical evidence of magma sediment hybridization indicative of an intense mingling process inferred to occur during the emplacement phase. The rheology of the soft, unconsolidated sediment controls and explains the various intrusion shapes and dimensions. Numerical simulation results indicate that heat dissipation in this context is much less efficient, which in turn considerably decreases the amount of thermogenic gas mobilized through thermal cracking in the contact aureole of sills. Additionally, we observe that hydrothermal pipe systems established during the cooling phase of sill emplacement can remain active at moderate- to low-temperature state after the heat of the sill has vanished. Using 2D seismic information and IODP drilling results, we were able to reconstruct the 3D structure of the sill at depth. It is funnel-shaped and roots in a depth where geothermal fluids can ascend from. The temperature found at these depths is consistent with the background geothermal gradient, suggesting that the large heat flow anomaly found at Hole U1548C is the mere expression of the active hydrothermal circulation fuelled by deeply sourced geothermal fluids.These potentially long-lasting hydrothermal systems provide preferable temperature and energetic conditions for microbial activity to thrive, with mildly degraded petroleum components from below and water recharge from above. Moreover, evidence indicates that the sill at Site U1547 is non-unique at the scale of the Guaymas Basin. How many of these catabolic reactors form at the early rifting phase? Can this process perhaps trigger peaks in subsurface biomass production associated with new continental margin formation? Our research heralds the dawn of a new paradigm. We suggest that in the context of a nascent ocean, sill emplacement in the first 500 m of sediments may power life instead of suppressing it.

Magma emplacement in basin sediments at shallow levels initiates a plethora of processes, proceeding both simultaneously and sequential, and on variable length scales. On the grain scale, uptake and heating of sediment and pore fluids during magma emplacement, as well as the fractionation of a highly mobile fluid phase upon crystallization induce distinct rock microfabrics. IODP Expedition 385 drilled through the shallow sills emplaced in the active rift of the Guaymas Basin, Gulf of California. Here we present first results of a high-resolution X-ray µ-CT survey on drill core material recovered from Hole U1546, covering a shallow basaltic sill emplaced within 300 m below the seafloor. Comprising sample material from just a few meters from top and bottom contacts, from the center of the ca. 75 m thick sill, and a distinctly gabbroic region in the upper third of the sill, several characteristic features of the rock microfabric have been observed. In general, 3D quantitative digital image analysis of the porosity matches the trend determined by onboard moisture and density analyses. Detailed size and shape analysis reveal a bimodal distribution of the pores near the sill margins: Near the top contact, porosity is constituted by small interstitial pores and large spherical vesicles; Near the bottom contact, scarce pores comprise minute interstitial voids and dendritic cavities within granular concretions. While in the center layer of the sill pores are minuscule, porosity within the gabbroic region occurs as almost mm-sized interstitial cavities. The spherically-shaped large vesicles near the top contact feature a complex history: Ductile environment is required in the course of formation, and subsequent precipitation of zeolite or/and calcite can be observed. In places, iron sulfide is present near or at the vesicle walls. In addition, consideration of the grain phase allows further constraints. While plagioclase phenocrysts are abundant throughout the entire sill thickness, grain sizes of matrix pyroxenes and plagioclase near the center are larger than near the contact. In the gabbroic region the presence of hornblende is indicative of a water content of 2 to 3 wt.%. The induced lowering of the solidus temperatures in this region explains why very large crystal sizes are allowed to develop morphologies of pyroxene and plagioclase intergrowth resulting in a coarser gabbroic texture.

Dissolution rates of porous crystalline materials reflect the superposition of transport and surface control, mainly via the parameters saturation of the ambient fluid and distribution of surface energy. As a result, reacting surfaces evolve over time showing a heterogeneous distribution of surface rates. The spatiotemporal heterogeneity of surface reaction rates is analyzed using the rate map and rate spectra concept. Here, we quantify the dissolution rate variability covering the nm- to mm-scale of dissolving single-crystal and polycrystalline calcite samples, using a combined approach of X-ray micro-computed tomography (µ-CT) and vertical scanning interferometry (VSI). The dissolution experiments cover reaction periods from 15 minutes up to 54 days. The observed rate ranges are remarkably consistent over the entire reaction period but include a variability of about two orders of magnitude (10-9 - 3 * 10-7 mol m-2 s-1). The rate map data underscore the concurrent and superimposing impact of surface- vs. fluid flow controlled rate portions. The impact of fluid flow on reactivity at the mm-scale in the transport-controlled system is confirmed by 2-D reactive transport modeling. The sub-mm spatial heterogeneity of low vs. high reactivity surface portions of polycrystalline calcite is clearly below the mean crystal size. This suggests the dominant impact of highly reactive surface portions irrespective of the orientation of larger crystals on the overall surface reactivity. Correspondingly, the overall range of intrinsic reactivity heterogeneity as observed using singly crystal material is not further expanded for polycrystalline material. As a general conclusion, numerical reactive transport concepts would benefit from the implementation of a reactivity term resembling the experimentally observed existence of multiple rate components.

Crystal morphologies are essential for deciphering the reaction history of igneous and metamorphic rocks because they often record the interplay between nucleation and growth rates controlled by the departure from equilibrium. Here, we report an exceptional record of the morphological transition of olivine formed during subduction metamorphism and high-pressure dehydration of antigorite-serpentinite to prograde chlorite-harzburgite in the Almirez ultramafic massif (Nevado–Filabride Complex, Betic Cordillera, SE Spain). In this massif, rare varied-textured chlorite-harzburgite (olivine+enstantite+chlorite+oxides) —formed after high–P dehydration of antigorite-serpentinite— exhibits large olivine porphyroblasts made up of rounded cores mantled by coronas of tabular olivine grains, similar to single tabular olivines occurring in the matrix. The correlative X-ray μ-CT and EBSD study of two varied-textured chlorite-harzburgite samples show that tabular olivine in coronas is tabular on (100)Ol with c > b >> a, and grew in nearly the same crystallographic orientation as the rounded olivine cores of the porphyroblast. Quantitative textural analysis and mass balance indicate that varied-textured chlorite-harzburgite is the result of a two-stage nucleation and growth of olivine during the progress of the high–P dehydration of antigorite-serpentinite to chlorite-harzburgite reaction. The first stage occurred under a low affinity (ΔGr) and affinity rate (ΔGr/dt) of the antigorite dehydration reaction that resulted in a low time-integrated nucleation rate and isotropic growth of olivine, forming rounded olivine porphyroblasts. With further progress of the dehydration reaction, a second stage of relatively higher affinity and affinity rate resulted in a higher time-integrated nucleation rate of olivine coeval with a shift from isotropic to anisotropic olivine growth, leading to tabular olivines. The two-stage evolution resulted in olivine porphyroblasts made up of rounded cores mantled by coronas of tabular olivine grains characteristic of varied-texture chlorite-harzburgite. Although a switch to anisotropic tabular olivine in the second stage is consistent with the relative increase in the affinity and affinity rate, these changes cannot solely account for the growth of Almirez olivine tabular on (100). Tabular olivines in komatiites and other igneous rocks are tabular on (010)Ol with either a > c >> b, or a ≈ c > > b, in agreement with experimentally determined growth rates of olivine phenocrysts under moderate to high undercooling and cooling rates. On the other hand, olivine tabular on (100) is expected in the presence of highly polymerized fluids where inhibited growth of the olivine (100) and (010) interfaces occurs, respectively, due to dissociative and molecular adsorption of water monolayers. Rounded and tabular olivines in Almirez varied-textured chlorite-harzburgite show differing trace element compositions that we interpret as due to the infiltration of external fluids during antigorite dehydration. Isothermal infiltration of highly polymerized fluids would explain the shift in the affinity and affinity rate of the antigorite dehydration reaction, as well as the olivine morphology tabular on (100) due to the inhibited growth on the (100) and, to a lesser extent, (010). Our study shows that surface-active molecules may play an essential role in shaping the morphology of growing crystals during fluid-present metamorphic crystallization.