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Abstract We report the formation of minerals from the tochilinite-valleriite group (TVG) during laboratory serpentinization experiments conducted at 300 and 328 °C. Minerals in the TVG are composed of a mixture of sulfide and hydroxide layers that can contain variable proportions of Fe, Mg, Cu, Ni, and other cations in both layers. Members of this group have been observed as accessory minerals in several serpentinites, and have also been observed in association with serpentine minerals in meteorites. To our knowledge, however, TVG minerals have not previously been identified as reaction products during laboratory simulation of serpentinization. The serpentinization experiments reacted olivine with artificial seawater containing 34S-labeled sulfate, with a small amount of solid FeS also added to the 300 °C experiment. In both experiments, the predominant reaction products were chrysotile serpentine, brucite, and magnetite. At 300 °C, these major products were accompanied by trace amounts of the Ni-bearing TVG member haapalaite, Ni,Fe-sulfide (likely pentlandite), and anhydrite. At 328 °C, valleriite occurs rather than haapalaite and the accompanying Ni,Fe-sulfide is proportionally more enriched in Ni. Reduction of sulfate by H2 produced during serpentinization evidently provided a source of reduced S that contributed to formation of the TVG minerals and Ni,Fe-sulfides. The results provide new constraints on the conditions that allow precipitation of tochilinite-valleriite group minerals in natural serpentinites. 

Abstract The minerals carrying the magnetic remanence in geological samples are commonly a solid solution series of iron‐titanium spinels known as titanomagnetites. Despite the range of possible compositions within this series, micromagnetic studies that characterize the magnetic domain structures present in these minerals have typically focused on magnetite. No studies systematically comparing the domain‐states present in titanomagnetites have been undertaken since the discovery of the single vortex (SV) structure and the advent of modern micromagnetism. The magnetic properties of the titanomagnetite series are known to vary strongly with composition, which may influence the domain states present in these minerals, and therefore the magnetic stability of the samples bearing them. We present results from micromagnetic simulations of titanomagnetite ellipsoids of varying shape and composition to find the size ranges of the single domain (SD) and SV structures. These size ranges overlap, allowing for regions where the SD and SV structures are both available. These regions are of interest as they may lead to magnetic instability and “partial thermal remanent magnetization (pTRM) tails” in paleointensity experiments. We find that although this SD + SV zone occupies a narrow range of sizes for equidimensional magnetite, it is widest for intermediate (TM30‐40) titanomagnetite compositions, and increases for both oblate and prolate particles, with some compositions and sizes having an SD + SV zone up to 100s of nm wide. Our results help to explain the prevalence of pTRM tail‐like behavior in paleointensity experiments. They also highlight regions of particles with unusual domain states to target for further investigation into the definitive mechanism behind paleointensity failure. 

SUMMARY The Verwey transition in magnetite is a crystallographic phase transition occurring in the temperature range 80–125 K and depends on stoichiometry and cation substitution, which may in turn serve as an indicator of the conditions under which magnetite was formed or altered in nature. We have analysed the distribution of Verwey transition temperatures (TV) in a large set of samples (N = 1110) from a wide variety of rocks, sediments, and other natural and synthetic materials containing magnetite, mined from the database of the Institute for Rock Magnetism and from published studies. The analysis is restricted to measurements of remanence while warming through the transition from which TV was determined by the derivative method. Our analysis showed that the TV distribution exhibited a generally bimodal distribution of Verwey transition temperatures, both for the entire data set and for almost all of the lithological subsets. There is a sharp peak for values in the range 118–120 K, and a broad, relatively flat or polymodal distribution from about 98 to 118 K. The upper end of the distribution was sharp, with only a few values exceeding 124 K, and the tail on the lower end extended down to about 80 K. Virtually all of the sample types exhibited polymodal distributions, almost always with one peak near 120 K, and with one or more additional peaks at lower temperatures. Biogenic magnetites produced by magnetotactic bacteria had the lowest modal value of TV (100 K). Loesses (103.5 K) and igneous extrusives (102.5 K) also had low modal transition temperatures and distributions with dominant low-TV peaks. Lithological groups with the highest modal transition temperatures were modern soils (119.5 K), silicate minerals with exsolved magnetite (119 K) and sedimentary rocks (119 K). Numerical experiments confirmed that the derivative method for the determination of TV was reasonably robust and that the observed distributions cannot be explained as an artefact related to the determination of TV from individual thermomagnetic runs but rather is a general characteristic of natural magnetites. The results provide context for studies that interpret TV in particular samples in terms of natural processes or conditions during formation or alteration of magnetite. 

Fires are an integral part of many terrestrial ecosystems and have a strong impact on soil properties. While reports of topsoil magnetic enhancement after fires vary widely, recent evidence suggests that plant ashes provide the most significant source of magnetic enhancement after burning. To investigate the magnetic properties of burnt plant material, samples of individual plant species from Iceland and Germany were cleaned and combusted at various temperatures prior to rock magnetic and geochemical characterization. Mass-normalized saturation magnetization values for burnt plant residues increase with the extent of burning in nearly all samples. However, when normalized to the loss on ignition, fewer than half of ash and charcoal samples display magnetic enhancement relative to intact plant material. Thus, while magnetic mineral concentrations generally increase, changes in the total amount of magnetic material are much more variable. Elemental analyses of Icelandic samples reveal that both total plant Fe and saturation magnetization are strongly correlated with Ti and Al, indicating that most of the Fe-bearing magnetic phases originate from inorganic material such as soil and atmospheric dust. Electron microscopy confirmed that inorganic particulate matter remains on most plant surfaces after cleaning. Plants with more textured leaf surfaces retain more dust, and ash from these samples tend to exhibit higher saturation magnetization and metal concentrations. Magnetic properties of plant ash therefore result from the thermal transformation of Fe in both organic compounds and inorganic particulate matter, which become concentrated on a mass basis when organic matter is combusted. These results indicate that the soil magnetic response to burning will vary among sites and regions as a function of 1) fire intensity, 2) the local composition of dust and soil particles on leaf surfaces, and 3) vegetation type and consequent differences in leaf morphologies. 

A series of three laboratory experiments were conducted to investigate how pH affects reaction pathways and rates during serpentinization. Two experiments were conducted under strongly alkaline conditions using olivine as reactant at 200 and 230°C, and the results were compared with previous studies performed using the same reactants and methods at more neutral pH. For both experiments, higher pH resulted in more rapid serpentinization of the olivine and generation of larger amounts of H 2 for comparable reaction times. Proportionally greater amounts of Fe were partitioned into brucite and chrysotile and less into magnetite in the experiments conducted at higher pH. In a third experiment, alkaline fluids were injected into an ongoing experiment containing olivine and orthopyroxene to raise the pH from circumneutral to strongly alkaline conditions. Increasing the pH of the olivine-orthopyroxene experiment resulted in an immediate and steep increase in H 2 production, and led to far more extensive reaction of the primary minerals compared to a similar experiment conducted under more neutral conditions. The results suggest that the development of strongly alkaline conditions in actively serpentinizing systems promotes increased rates of reaction and H 2 production, enhancing the flux of H 2 available to support biological activity in these environments. This article is part of a discussion meeting issue ‘Serpentinite in the Earth System’.