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Diamonds growing in the Earth’s mantle often trap inclusions of fluids that are highly saline in composition. These fluids are thought to emerge from deep in subduction zones and may also be involved in the generation of some of the kimberlite magmas. However, the source of these fluids and the mechanism of their transport into the mantle lithosphere are unresolved. Here, we present experimental results showing that alkali chlorides are stable solid phases in the mantle lithosphere below 110 km. These alkali chlorides are formed by the reaction of subducted marine sediments with peridotite and show identical K/Na ratios to fluid inclusions in diamond. At temperatures >1100°C and low pressures, the chlorides are unstable; here, potassium is accommodated in mica and melt. The reaction of subducted sediments with peridotite explains the occurrence of Mg carbonates and the highly saline fluids found in diamonds and in chlorine-enriched kimberlite magmas.
Metasomatic reaction zones between mafic and ultramafic rocks exhumed from subduction zones provide a window into mass-transfer processes at high pressure. However, accurate interpretation of the rock record requires distinguishing high-pressure metasomatic processes from inherited oceanic signatures prior to subduction. We integrated constraints from bulk-rock geochemical compositions and petrophysical properties, mineral chemistry, and thermodynamic modeling to understand the formation of reaction zones between juxtaposed metagabbro and serpentinite as exemplified by the Voltri Massif (Ligurian Alps, Italy). Distinct zones of variably metasomatized metagabbro are dominated by chlorite, amphibole, clinopyroxene, epidote, rutile, ilmenite, and titanite between serpentinite and eclogitic metagabbro. Whereas the precursor serpentinite and oxide gabbro formed and were likely already in contact in an oceanic setting, the reaction zones formed by diffusional Mg-metasomatism between the two rocks from prograde to peak, to retrograde conditions in a subduction zone. Metasomatism of mafic rocks by Mg-rich fluids that previously equilibrated with serpentinite could be widespread along the subduction interface, within the subducted slab, and the mantle wedge. Furthermore, the models predict that talc formation by Si-metasomatism of serpentinite in subduction zones is limited by pressure-dependent increase in the silica activity buffered by the serpentine-talc equilibrium. Elevated activities of aqueous Ca and Al species would also favor the formation of chlorite and garnet. Accordingly, unusual conditions or processes would be required to stabilize abundant talc at high P-T conditions. Alternatively, a different set of mineral assemblages, such as serpentine- or chlorite-rich rocks, may be controlling the coupling-decoupling transition of the plate interface.
Talc formation via silica-metasomatism of ultramafic rocks is believed to play key roles in subduction zone processes. Yet, the conditions of talc formation remain poorly constrained. We used thermodynamic reaction-path models to assess the formation of talc at the slab-mantle interface and show that it is restricted to a limited set of pressure–temperature conditions, protolith, and fluid compositions. In contrast, our models predict that chlorite formation is ubiquitous at conditions relevant to the slab-mantle interface of subduction zones. The scarcity of talc and abundance of chlorite is evident in the rock record of exhumed subduction zone terranes. Talc formation during Si-metasomatism may thus play a more limited role in volatile cycling, strain localization, and in controlling the decoupling-coupling transition of the plate interface. Conversely, the observed and predicted ubiquity of chlorite corroborates its prominent role in slab-mantle interface processes that previous studies attributed to talc.
Key Points:
Limited talc formation by Si-metasomatism of ultramafic rocks in subduction zones
Chlorite formation is likely pervasive at the slab-mantle interface
Preferential formation of chlorite has wide-ranging chemical and physical implications for subduction zone processes
Plain Language Summary: In subduction zones, talc can form during chemical reactions of mantle rocks with silica-enriched fluids at the interface between descending oceanic plates and the overriding mantle. Its formation and distribution in subduction zones are believed to affect the volatile budget, rheological properties, and the down-dip limit of the decoupling of the slab-mantle interface. Therefore, illuminating the conditions that facilitate talc formation at high pressure-temperature conditions is key in assessing its roles in fundamental subduction zone processes. Using thermodynamic reaction-path models, we show that the formation of talc at the slab-mantle interface is restricted to a limited set of environmental conditions, because its formation is highly sensitive to the compositions of the mantle rocks and reactant fluids. Contrary to common belief, talc is unlikely to form in high abundance in ultramafic rocks metasomatized by Si-rich slab-derived fluids. Rather, our models predict the ubiquitous formation of chlorite along with other silicate minerals during Si-metasomatism due to the competing effects from other dissolved components that favor their formation over talc. This study calls into question the importance of talc during Si-metasomatism in subduction zones but highlights the more predominant role of chlorite.
Garnet xenocrysts from kimberlites provide unique insights into the composition, structure and evolution of the subcontinental lithospheric mantle (SCLM). For example, different metasomatic events in the SCLM are reflected in compositional differences between garnet xenocrysts. As mantle metasomatism largely controls the physical and chemical properties of the SCLM, it exerts first order control over the genesis of kimberlitic magmas and diamond formation. However, dating mantle lithologies and processes is complicated by high ambient temperatures that allow the equilibration of most isotopic systems up to the time of kimberlite eruption. As a consequence, the temporal connection between metasomatic events in the mantle and kimberlite genesis is commonly ambiguous.
In this study, we applied LA-ICPMS U-Pb dating to 43 harzburgitic, lherzolithic and megacrystic garnet xenocrysts from the ~376 Ma diamondiferous V. Grib kimberlite, Russia, in order to investigate the link between different types of mantle metasomatism and kimberlite genesis.
Our results indicate that, with two possible exceptions, only harzburgitic garnet overlaps in age with the kimberlite eruption, whereas lherzolitic and megacrystic garnet crystals are ~20 to 130 million years older. Furthermore, garnet U-Pb ages and Ni-in-garnet temperatures of ~820 to 1200 °C do not correlate. This, and the high closure temperature of U-Pb in garnet (≥900 °C) suggests that the garnet U-Pb ages indeed reflect metasomatic events in the SCLM. However, the U-Pb ages could also reflect cooling ages. In this case, the metasomatic events recorded in the garnet crystals must still have occurred up to ~130 million years prior to the eruption of the V. Grib kimberlite.
These findings have far-reaching implications for the genesis of (diamondiferous) kimberlites, as they clearly show that the time lag between metasomatic events in the SCLM, as recorded in kimberlitic garnet xenocrysts, and kimberlite eruption may extend to tens of millions of years.
Fossil records of early solar irradiation and cosmolocation of the CAI factory: a reappraisal
(2021)
Calcium-aluminum–rich inclusions (CAIs) in meteorites carry crucial information about the environmental conditions of the nascent Solar System prior to planet formation. Based on models of 50V–10Be co-production by in-situ irradiation, CAIs are considered to have formed within ~0.1 AU from the proto-Sun. Here, we present vanadium (V) and strontium (Sr) isotopic co-variations in fine- and coarse-grained CAIs and demonstrate that kinetic isotope effects during partial condensation and evaporation best explain V isotope anomalies previously attributed to solar particle irradiation. We also report initial excesses of 10Be and argue that CV CAIs possess essentially a homogeneous level of 10Be, inherited during their formation. Based on numerical modeling of 50V–10Be co-production by irradiation, we show that CAI formation during protoplanetary disk build-up likely occurred at greater heliocentric distances than previously considered, up to planet-forming regions (~1AU), where solar particle fluxes were sufficiently low to avoid substantial in-situ irradiation of CAIs.
Chloritoid and kyanite coexist in metapelites from the high-pressure/low-temperature Massa Unit in the Alpi Apuane metamorphic complex (Northern Apennines, Italy). The composition of chloritoid is extremely variable throughout the Massa Unit. Fe-chloritoid occurs in association with hematite-free, graphite-bearing schists, whereas strongly zoned Fe-Mg chloritoid is found with hematite and kyanite. We investigated the effect of different bulk Fe2O3 contents in controlling chloritoid composition through phase equilibria modelling of four selected samples, representative of the different chloritoid-bearing parageneses found in the Massa Unit. The ferric iron content, measured through wet chemical titration, ranges from 0 (graphite-chloritoid schist) to 73% of the total iron (hematite-chloritoid schist). We show that Mg-rich chloritoid compositions and stability of kyanite at greenschist to blueschist facies conditions can be reproduced in the MnO–Na2O–K2O–FeO–MgO–Al2O3–SiO2–H2O–TiO2–O (MnNKFMASHTO) chemical system only considering the presence of significant amounts of ferric iron as part of the bulk composition. The stabilization of kyanite at lower grade is directly linked to the presence of Fe2O3, which renders the reactive bulk rock composition effectively enriched in Al2O3 with respect to Fe and Mg. We also document that high Fe2O3 contents exacerbate the effect of chloritoid fractionation, producing strongly zoned Fe-Mg-chloritoid grains. Finally, the P–T modelling of the Massa Units performed in this study allows, for the first time, the recognition of a two-stage evolution at peak conditions, with an earlier pressure peak (1.2–1.3 GPa at 350–400°C), and a later thermal peak (0.7–1.1 GPa at 440–480°C), compatible with subduction, underthrusting and exhumation of the Adria continental margin during growth of the Northern Apennine orogenic wedge.
The oxidation state of sulfur in slab fluids is controversial, with both dominantly oxidized and reduced species proposed. Here we use in situ X-ray absorption spectroscopy analysis of sulfur-in-apatite to monitor changes in the oxidation state of sulfur during high-P metasomatism by slab fluids in the subduction channel. Our samples include a 73 cm continuous transect of reaction zones between a metagabbroic eclogite block and serpentinite matrix from a mélange zone on the island of Syros, Greece. The block core consists of garnet, omphacite, phengite, paragonite, epidote-clinozoisite, and rutile. In this region, apatite is only observed as elongate inclusions in omphacite cores. From the core outwards micas are increasingly replaced by epidote-clinozoisite, garnets are smaller and more frequent, pyrite + bornite is observed as inclusions in recrystallized omphacite, and apatite is increasingly abundant in the matrix and inclusions in garnet. A major transition at 48 cm separates an assemblage of Ca-Na amphibole, omphacite, chlorite, pyrite, and apatite from the inner garnet-bearing eclogite assemblages. Omphacite disappears from the assemblage at ~56 cm and amphibole compositions sharply transition to tremolite at 59 cm. Finally, the assemblage tremolite + talc + pyrite is observed after ~70 cm.Apatites in the eclogite assemblages exclusively display S6+ peaks in their absorption spectra. This includes apatite inclusions in omphacite in the least altered lithology, as well as matrix apatite and isolated apatite inclusions in garnet in the outermost metasomatized eclogite zone. In the intermediate pyrite-rich (~1-5 vol %) amphibole + omphacite + chlorite zone, apatite displays a strong S1- absorption peak in most grains, with rare analyses showing mixed S1- and S6+. Finally, apatite in the outermost tremolite-bearing assemblages only displays a S6+ peak. The pyrite-rich zone at 48 cm occurs at the initial interface between the serpentinite matrix and eclogite block, characterized by a dramatic decrease in Na content and Mg#. Our data suggest that reduction of S6+ in infiltrating fluids to S1- in pyrite became focused as Fe diffused across the steep Mg# gradient, resulting in pyrite precipitation. In contrast, S reduction in the Mg-rich tremolite-dominant portions of the transect was limited by a lack of Fe, resulting in low modes of pyrite and fluid buffered S6+ in apatite. Finally, S6+-bearing apatite is also observed in reaction zone lithologies from elsewhere on Syros, suggesting our observations are not isolated.Two important conclusions are drawn from these data and observations: (1) In the case of Syros, slab fluids at eclogite-facies conditions carried oxidized S6+, and (2) The interaction of these fluids with eclogites composed of ferrous-Fe silicates resulted in extensive sulfide precipitation.
In subduction zones, sediments and hydrothermally altered oceanic crust, which together form part of the subducting slab, contribute to the chemical composition of lavas erupted at the surface to form volcanic arcs. Transport of this material from the slab to the overlying mantle wedge is thought to involve discreet melts and fluids that are released from various portions of the slab. We use a meta-analysis of geochemical data from eight globally representative arcs to show that melts and fluids from individual slab components cannot be responsible for the formation of arc lavas. Instead, the data are compatible with models that first invoke physical mixing of slab components and the mantle wedge, widely referred to as high-pressure mélange, before arc magmas are generated.
Sulfur in the slab: a sulfur-isotopes and thermodynamic-modeling perspective from exhumed terranes
(2022)
Sulfur is a key element in the subduction zone-volcanic arc system; however, the mechanism(s) that recycle sulfur from the slab into the overlying volcanic arc are debated. Here we summarize recent advances in quantifying this component of the deep sulfur cycle. First, primary metamorphic or inherited sulfides in oceanic-type eclogites are only rarely observed as inclusions and are typically absent from the rock matrix. Additionally, sulfides are relatively common in rocks metasomatized at the slab-mantle interface by slab-derived fluids during exhumation. Combined, these two observations suggest that sulfur loss from subducted mafic crust is relatively efficient. Thermodynamic modeling in Perple_X using the Holland and Powell (2011) database combined with the Deep Earth Water model suggests that the efficiency and speciation of sulfur loss varies depending on the degree of seafloor alteration prior to subduction and the geothermal gradient of the slab. In relatively cold subduction zones, such as Honshu, slab-fluids derived from subducted mafic crust are predicted to exhibit elevated concentrations of HSO4-, SO42-, HSO3-, and CaSO4(aq), whereas hot subduction zones, such as Cascadia, are predicted to produce slab fluids enriched in HS- and H2S at lower pressures. The oxidation of sulfur expelled from subducted pyrite is balanced by the reduction of Fe3+ to Fe2+, consistent with the low Fe3+/SFe of exhumed eclogites relative to blueschists and altered oceanic crust. Where oxidized S-bearing fluids are produced, they are anticipated to interact with more reduced rocks at the slab-mantle interface and within the mantle wedge, resulting in sulfide precipitation and significant isotopic fractionation. The δ34S values of slab fluids are estimated to fall between -11 and +8 ‰. Rayleigh fractionation during progressive fluid-rock interaction results in fractionations of tens of per mil as oxidized species are depleted and sulfides are precipitated, resulting in δ34S values of sulfides that easily span the -21.7 to +13.9 ‰ range observed in metasomatic sulfides in exhumed high-pressure rocks. However, in subduction zones where reduced species prevail, the S isotopic signature of slab fluids is expected to reflect their source and will exhibit a narrower range in δ34S values. As a result, the δ34S values measured in arc magmas may not always be a reliable indicator of the contribution of different components of the slab, such as sediments vs. AOC. Additionally, the impact of S recycling on the oxygen fugacity of arc magmas is expected to vary both spatially and temporally throughout Earth history.
This chapter reviews the boron isotopic composition of the ocean floor, including pristine igneous oceanic crust such as mid-ocean ridge basalts and ocean island basalts and their implications for the B isotopic composition of the mantle. The chapter further discusses the B isotopic effects of assimilation of altered crustal materials in mantle-derived magmas. The systematics of seawater alteration on oceanic rocks are discussed, including sediments, igneous crust and serpentinization of ultramafic rocks and the respective marine hydrothermal vent fluids. The chapter concludes with a discussion of the secular evolution of the B isotopic composition of seawater.
Titanite is a potentially powerful U–Pb petrochronometer that may record metamorphism, metasomatism, and deformation. Titanite may also incorporate significant inherited Pb, which may lead to inaccurate and geologically ambiguous U–Pb dates if a proper correction is not or cannot be applied. Here, we present laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS)-derived titanite U–Pb dates and trace element concentrations for two banded calcsilicate gneisses from south-central Maine, USA (SSP18-1A and SSP18-1B). Single spot common Pb-corrected dates range from 400 to 280 Ma with ±12–20 Ma propagated 2SE. Titanite grains in sample SSP18-1B exhibit regular core-to-rim variations in texture, composition, and date. We identify four titanite populations: (1) 397 ± 5 Ma (95% CL) low Y + HREE cores and mottled grains, (2) 370 ± 7 Ma high Y + REE mantles and cores, (3) 342 ± 6 Ma cores with high Y + REE and no Eu anomaly, and (4) 295 ± 6 Ma LREE-depleted rims. We interpret the increase in titanite Y + HREE between ca. 397 and ca. 370 Ma to constrain the timing of diopside fracturing and recrystallization and amphibole breakdown. Apparent Zr-in-titanite temperatures (803 ± 36°C at 0.5 ± 0.2 GPa) and increased XDi suggest a thermal maximum at ca. 370 Ma. Population 3 domains dated to ca. 342 Ma exhibit no Eu anomaly and are observed only in compositional bands dominated by diopside (>80 vol%), suggesting limited equilibrium between titanite and plagioclase. Finally, low LREE and high U/Th in Population 4 titanite dates the formation of hydrous phases, such as allanite, during high XH2O fluid infiltration at ca. 295 Ma. In contrast to the well-defined date–composition–texture relationships observed for titanite from SSP18-1B, titanite grains from sample SSP18-1A exhibit complex zoning patterns and little correlation between texture, composition, and date. We hypothesize that the incorporation of variable amounts of radiogenic Pb from dissolved titanite into recrystallized domains resulted in mixed dates spanning 380–330 Ma. Although titanite may reliably record multiple phases of metamorphism, these data highlight the importance of considering U–Pb data along with chemical and textural data to screen for inherited radiogenic Pb.
Reliable identification of chondrules, calcium-aluminum-rich inclusions (CAIs), carbonate grains, and Ca-phosphate grains at depth within untouched, unprepared chondritic samples by a nondestructive analytical method, such as synchrotron X-ray fluorescence (SXRF) computed tomography (CT), is an essential first step before intrusive analytical and sample preparation methods are performed. The detection of a local Ca-enrichment could indicate the presence of such a component, all of which contain Ca as major element and/or Ca-bearing minerals, allowing it to be precisely located at depth within a sample. However, the depth limitation from which Ca-K fluorescence can travel through a chondrite sample (e.g., ∼115 µm through material of 1.5 g cm−3) to XRF detectors leaves many Ca-bearing components undetected at deeper depths. In comparison, Sr-K lines travel much greater distances (∼1700 µm) through the same sample density and are, thus, detected from much greater depths. Here, we demonstrate a clear, positive, and preferential correlation between Ca and Sr and conclude that Sr-detection can be used as proxy for the presence of Ca (and, thus, Ca-bearing components) throughout mm-sized samples of carbonaceous chondritic material. This has valuable implications, especially for sample return missions from carbonaceous C-type asteroids, such as Ryugu or Bennu. Reliable localization, identification, and targeted analysis by SXRF of Ca-bearing chondrules, CAIs, and carbonates at depth within untouched, unprepared samples in the initial stages of a multianalysis investigation insures the valuable information they hold of pre- and post-accretion processes in the early solar system is neither corrupted nor destroyed in subsequent processing and analyses.
Questions: Both species turnover and intraspecific trait variation can affect plant assemblage dynamics along environmental gradients. Here, we asked how community assemblage patterns in relation to species turnover and intraspecific variation differ between endemic and non-endemic species. We hypothesized that endemic species show lower intraspecific variation than non-endemic species because they tend to have high rates of in situ speciation, whereas non-endemic species are expected to have a larger gene pool and higher phenotypic plasticity.
Location: La Palma, Canary Islands.
Methods: We established 44 sampling sites along a directional gradient of precipitation, heat load, soil nitrogen, phosphorus and pH. Along this gradient, we estimated species abundances and measured three traits (plant height, leaf area and leaf thickness) on perennial endemic and non-endemic plant species. In total, we recorded traits for 1,223 plant individuals of 43 species. Subsequently, we calculated community-weighted mean traits to measure the relative contribution of species turnover, intraspecific variation and their covariation along the analysed gradient.
Results: The contribution of intraspecific variation to total variation was similar in endemic and non-endemic assemblages. For plant height, intraspecific variation explained roughly as much variation as species turnover. For leaf area and leaf thickness, intraspecific variation explained almost no variation. Species turnover effects mainly drove trait responses along the environmental gradient, but intraspecific variation was important for responses in leaf area to precipitation.
Conclusions: Despite their distinct evolutionary history, endemic and non-endemic plant assemblages show similar patterns in species turnover and intraspecific variation. Our results indicate that species turnover is the main component of trait variation in the underlying study system. However, intraspecific variation can increase individual species’ fitness in response to precipitation. Overall, our study challenges the theory that intraspecific trait variation is more important for the establishment of non-endemic species compared with endemic species.
Positive plant–plant interactions are thought to drive vegetation patterns in harsh environments, such as semi-arid areas. According to the stress-gradient hypothesis (SGH), the role of positive interactions between species (facilitation) is expected to increase with harshness, predicting associated variation in species composition along environmental gradients. However, the relation between stress and facilitation along environmental gradients is debated. Furthermore, differentiating facilitative interactions from other underlying mechanisms, such as microtopographic heterogeneity, is not trivial. We analysed the spatial co-occurrence relationships of vascular plant species that form patchy vegetation in arid lapilli fields (tephra) from recent volcanic eruptions on La Palma, Canary Islands. Assuming a harshness gradient negatively correlated with elevation because the lower elevations are more arid and water availability is considered the most limiting resource, and that an outcome of facilitation is plants co-occurring in the same patch, from the SGH we expected a greater degree of co-occurrence at lower elevation. We tested this at both the species and the individual plant level. We analysed the species composition of 1277 shrubby vegetation patches at 64 different sampling points, ranging from the coast to around 700 m a.s.l. Patch morphology and microtopographic heterogeneity variables were also measured, to account for their potential effects on the species composition of patches. We used generalized linear models and generalized mixed-effects models to analyse species richness, number of individuals in patches and percentage of patches with positive co-occurrences, and a pairwise co-occurrence analysis combined with a graphical network analysis to reveal positive links between 13 of the species. We found that the percentage of patches with positive co-occurrences increased at higher elevations, in contrast to the predictions of the SGH, but in accordance with a refined stress-gradient hypothesis for arid sites, in which characteristics of the interacting species are incorporated.
This thesis presents the experimental and numerical analysis of seismic waves that are produced by wind farms. With the aim to develop renewable energies rapidly, the number of wind turbines has been increased in recent years. Ground motions induced by their operation can be observed by seismometers several kilometers away. Hence, the seismic noise level can be significantly increased at the seismic station. Therefore, this study combines long-term experiments and numerical simulations to improve the understanding of the seismic wavefields emitted by complete wind farms and to advance the prediction of signal amplitudes.
Firstly, wind-turbine induced signals that are measured at a small wind farm close to Würzburg (Germany) are correlated with the operational data of the turbines. The frequency-dependent decay of signal amplitudes with distance from the wind farm is modeled using an analytical method including the complex effects of interferences of the wavefields produced by the multiple wind turbines. Specific interference patterns significantly affect the wave propagation and therefore the signal amplitude in the far field of a wind farm. Since measurements inside the wind turbines show that the assumption of in-phase vibrating wind turbines is inappropriate, an approach to calculate representative seismic radiation patterns from multiple wind turbines, which allows the prediction of amplitudes in the far field of a complete wind farm, is proposed.
In a second study, signals with a frequency of 1.15 Hz, produced by the Weilrod wind farm (north of Frankfurt, Germany) are observed at the seismological observatory TNS (Taunus), which is located at a distance of 11 km from the wind farm. The propagation of the wavefield emitted by the wind farm is numerically modeled in 3D, using the spectral element method. It is shown that topographic effects can cause local signal amplitude reductions, but also signal amplification along the travel path of the seismic wave. The comparison of simulations with and without topography reveals that the reduction and amplification are spatially linked to the shape of the topography, which could be an explanation for the relatively high signal amplitude observed at TNS.
Finally, the reduction of the impact of wind turbines on seismic measurements using borehole installations is studied using 2D numerical models. Possible effects of the seismic velocity, attenuation, and layering of the subsurface are demonstrated. Results show that a borehole can be very effective in reducing the observed high-frequency signals emitted by wind turbines. However, a borehole might not be beneficial if signals with frequencies of about 1 Hz (or lower) are of interest, due significant wavelength-dependent effects. The estimations of depth-dependent amplitudes with a layered subsurface are validated with existing data from wind-turbine-induced signals measured at the top and bottom of two boreholes.
The experimental analysis of measurements conducted at wind farms and the advances of modeling such signals improve the understanding of the propagation of wind-farm induced seismic wave fields. Furthermore, the methods developed in this work have a high potential of universal application to the prediction of signal amplitudes at seismometers close to wind farms with arbitrary layout and geographic location.
Nontarget screening exhibits a seasonal cycle of PM2.5 organic aerosol composition in Beijing
(2022)
The molecular composition of atmospheric particulate matter (PM) in the urban environment is complex, and it remains a challenge to identify its sources and formation pathways. Here, we report the seasonal variation of the molecular composition of organic aerosols (OA), based on 172 PM2.5 filter samples collected in Beijing, China, from February 2018 to March 2019. We applied a hierarchical cluster analysis (HCA) on a large nontarget-screening data set and found a strong seasonal difference in the OA chemical composition. Molecular fingerprints of the major compound clusters exhibit a unique molecular pattern in the Van Krevelen-space. We found that summer OA in Beijing features a higher degree of oxidation and a higher proportion of organosulfates (OSs) in comparison to OA during wintertime, which exhibits a high contribution from (nitro-)aromatic compounds. OSs appeared with a high intensity in summer-haze conditions, indicating the importance of anthropogenic enhancement of secondary OA in summer Beijing. Furthermore, we quantified the contribution of the four main compound clusters to total OA using surrogate standards. With this approach, we are able to explain a small fraction of the OA (∼11–14%) monitored by the Time-of-Flight Aerosol Chemical Speciation Monitor (ToF-ACSM). However, we observe a strong correlation between the sum of the quantified clusters and OA measured by the ToF-ACSM, indicating that the identified clusters represent the major variability of OA seasonal cycles. This study highlights the potential of using nontarget screening in combination with HCA for gaining a better understanding of the molecular composition and the origin of OA in the urban environment.
Vladimir Vernadsky's concept of living matter is central to his biogeochemistry, the science he founded. For several reasons, his original understanding of living matter is one of the most complex notions in the history of the life sciences. First, biogeochemistry is by definition an interdisciplinary enterprise that embraces biology, including evolutionary theory, geology, and chemistry, and combines them into a unique research program. Second, if understood in the original sense as used by Vernadsky, living matter is a concept built into idiosyncratic metaphysics constructed around the so-called principle of life's eternity. Third, the concept of living matter reflects the specificity of Vernadsky's sophisticated philosophy of science as he insisted that 'scientific thought' is a planetary phenomenon as well as a geological force. In our contribution, we will introduce Vernadsky's concept of living matter in its historical context. Accordingly, we will also give some chronology of Vernadsky's work related to the growth of his biosphere concept highlighting the 'Ukrainian' period as it is in this period that he intensively elaborated on the notion of living matter. This will be followed by his theory of living matter as it was formulated in his major works of the later period. We are going to locate the notion of living matter within Vernadsky's theoretical system and demonstrate that he regarded his theory of the living as an evolutionary theory complementary to that of Charles Darwin from the very beginning. Additionally, we will briefly present Vladimir Beklemishev's concept of 'geomerida' which he developed at approximately the same time as Vernadsky was elaborating on his 'living matter' to highlight the specificity of the latter's methodology.