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Evidence of hydrothermal activity is reported for the Mesozoic pre- and syn-rift successions of the western Adriatic palaeomargin of the Alpine Tethys, preserved in the Western Southalpine Domain (NW Italy). The products of hydrothermal processes are represented by vein and breccia cements, as well as dolomitization and silicification of the host rocks. In the eastern part of the study area, interpreted as part of the necking zone of the continental margin, Middle Triassic dolostones and Lower Jurassic sediments are crossed by veins and hydrofracturing breccias cemented by saddle dolomite. The precipitation of dolomite cements occurred within the stratigraphic succession close to the sediment–water interface. Despite the shallow burial depth, fluid inclusion microthermometry and clumped isotopes show that hydrothermal fluids were relatively hot (80–150°C). In the western part of the study area, interpreted as part of the hyperextended distal zone, a polyphase history of host-rock fracturing is recorded, with at least two generations of veins cemented by calcite, dolomite and quartz. Vein opening and cementation occurred at shallow burial depth around the time of deposition of the syn-rift clastic succession. Fluid inclusion microthermometry on both quartz and dolomite cements indicates a fluid temperature of 90–130°C, again pointing to hydrothermal fluids. Both in Fenera-Sostegno and Montalto Dora areas, O, C and Sr isotope values, coupled with fluid inclusion and clumped isotope data, indicate that hydrothermal fluids derived from seawater interacted with crustal rocks during hydrothermal circulation. Stratigraphic and petrographic evidence, and U–Pb dating of dolomitized clasts within syn-rift sediments, document that hydrothermal fluids circulated through sediments from the latest Triassic to the Toarcian, corresponding to the entire syn-rift evolution of the western portion of the Adriatic palaeomargin. The documented hydrothermal processes are temporally correlated with regional-scale thermal events that took place in the same time interval at deeper crustal levels.
National greenhouse gas inventories (GHGIs) are submitted annually to the United Nations Framework Convention on Climate Change (UNFCCC). They are estimated in compliance with Intergovernmental Panel on Climate Change (IPCC) methodological guidance using activity data, emission factors and facility-level measurements. For some sources, the outputs from these calculations are very uncertain. Inverse modelling techniques that use high-quality, long-term measurements of atmospheric gases have been developed to provide independent verification of national GHGIs. This is considered good practice by the IPCC as it helps national inventory compilers to verify reported emissions and to reduce emission uncertainty. Emission estimates from the InTEM (Inversion Technique for Emission Modelling) model are presented for the UK for the hydrofluorocarbons (HFCs) reported to the UNFCCC (HFC-125, HFC-134a, HFC-143a, HFC-152a, HFC-23, HFC-32, HFC-227ea, HFC-245fa, HFC-43-10mee and HFC-365mfc). These HFCs have high global warming potentials (GWPs), and the global background mole fractions of all but two are increasing, thus highlighting their relevance to the climate and a need for increasing the accuracy of emission estimation for regulatory purposes. This study presents evidence that the long-term annual increase in growth of HFC-134a has stopped and is now decreasing. For HFC-32 there is an early indication, its rapid global growth period has ended, and there is evidence that the annual increase in global growth for HFC-125 has slowed from 2018. The inverse modelling results indicate that the UK implementation of European Union regulation of HFC emissions has been successful in initiating a decline in UK emissions from 2018. Comparison of the total InTEM UK HFC emissions in 2020 with the average from 2009–2012 shows a drop of 35 %, indicating progress toward the target of a 79 % decrease in sales by 2030. The total InTEM HFC emission estimates (2008–2018) are on average 73 (62–83) % of, or 4.3 (2.7–5.9) Tg CO2-eq yr−1 lower than, the total HFC emission estimates from the UK GHGI. There are also significant discrepancies between the two estimates for the individual HFCs.
The impact of precipitation in shallow cumulus convection on the moisture variance and third-order moments of moisture is investigated with the help of large-eddy simulations. Three idealized simulations based on the Rain in Cumulus over the Ocean field experiment are analyzed: one nonprecipitating, on a smaller domain, and two precipitating cases, on a larger domain with different initial profiles of moisture. Results show that precipitation and the associated cloud organization lead to increased generation of higher-order moments (HOM) of moisture compared to the nonprecipitating case. To understand the physical mechanism and the role of individual processes in this increase, budgets of HOM of moisture are studied. Microphysics directly decreases the generation of HOM of moisture, but this effect is not dominant. The gradient production term is identified as the main source term in the HOM budgets. The influence of the gradient production term on moisture variance is further examined separately in cloud active and nonactive regions. The main contribution to the gradient production term comes from the smaller cloud active region because of the stronger moisture flux. Further analyses of the horizontal and vertical cross sections of moisture fluctuations show that the precipitation-induced downdrafts and updrafts are the main mechanism for the generation of moisture variance. The variance increase is linked to shallow dry downdraft regions with horizontal divergence in the subcloud layer, moist updrafts with horizontal convergence in the bulk cloud layer, and finally wider areas of horizontal divergence in the cloud inversion layer.
We combined biostratigraphical analyses, archaeological surveys, and Glacial Isostatic Adjustment (GIA) models to provide new insights into the relative sea-level evolution in the northeastern Aegean Sea (eastern Mediterranean). In this area, characterized by a very complex tectonic pattern, we produced a new typology of sea-level index point, based on the foraminiferal associations found in transgressive marine facies. Our results agree with the sea-level history previously produced in this region, therefore confirming the validity of this new type of index point. The expanded dataset presented in this paper further demonstrates a continuous Holocene RSL rise in this portion of the Aegean Sea. Comparing the new RSL record with the available geophysical predictions of sea-level evolution indicates that the crustal subsidence of the Samothraki Plateau and the North Aegean Trough played a major role in controlling millennial-scale sea-level evolution in the area. This major subsidence rate needs to be taken into account in the preparation of local future scenarios of sea-level rise in the coming decades.
The Weissert Event ~133 million years ago marked a profound global cooling that punctuated the Early Cretaceous greenhouse. We present modelling, high-resolution bulk organic carbon isotopes and chronostratigraphically calibrated sea surface temperature (SSTs) based on an organic paleothermometer (the TEX86 proxy), which capture the Weissert Event in the semi-enclosed Weddell Sea basin, offshore Antarctica (paleolatitude ~54 °S; paleowater depth ~500 meters). We document a ~3–4 °C drop in SST coinciding with the Weissert cold end, and converge the Weddell Sea data, climate simulations and available worldwide multi-proxy based temperature data towards one unifying solution providing a best-fit between all lines of evidence. The outcome confirms a 3.0 °C ( ±1.7 °C) global mean surface cooling across the Weissert Event, which translates into a ~40% drop in atmospheric pCO2 over a period of ~700 thousand years. Consistent with geologic evidence, this pCO2 drop favoured the potential build-up of local polar ice.
In partially molten regions inside the Earth, melt buoyancy may trigger upwelling of both solid and fluid phases, i.e., diapirism. If the melt is allowed to move separately with respect to the matrix, melt perturbations may evolve into solitary porosity waves. While diapirs may form on a wide range of scales, porosity waves are restricted to sizes of a few times the compaction length. Thus, the size of a partially molten perturbation in terms of compaction length controls whether material is dominantly transported by porosity waves or by diapirism. We study the transition from diapiric rise to solitary porosity waves by solving the two-phase flow equations of conservation of mass and momentum in 2D with porosity-dependent matrix viscosity. We systematically vary the initial size of a porosity perturbation from 1.8 to 120 times the compaction length. If the perturbation is of the order of a few compaction lengths, a single solitary wave will emerge, either with a positive or negative vertical matrix flux. If melt is not allowed to move separately to the matrix a diapir will emerge. In between these end members we observe a regime where the partially molten perturbation will split up into numerous solitary waves, whose phase velocity is so low compared to the Stokes velocity that the whole swarm of waves will ascend jointly as a diapir, just slowly elongating due to a higher amplitude main solitary wave. Only if the melt is not allowed to move separately to the matrix will no solitary waves build up, but as soon as two-phase flow is enabled solitary waves will eventually emerge. The required time to build them up increases nonlinearly with the perturbation radius in terms of compaction length and might be too long to allow for them in nature in many cases.
The analysis of charcoal fragments in peat and lake sediments is the most widely used approach to reconstruct past biomass burning. With a few exceptions, this method typically relies on the quantification of the total charcoal content of the sediment. To enhance charcoal analyses for the reconstruction of past fire regimes and make the method more relevant to studies of both plant evolution and fire management, the extraction of more information from charcoal particles is critical. Here, I used a muffle oven to burn seven fuel types comprising 17 species from boreal Siberia (near Teguldet village), which are also commonly found in the Northern Hemisphere, and built on published schemes to develop morphometric and finer diagnostic classifications of the experimentally charred particles. I then combined these results with those from fossil charcoal from a peat core taken from the same location (Ulukh-Chayakh mire) in order to demonstrate the relevance of these experiments to the fossil charcoal records. Results show that graminoids, Sphagnum, and wood (trunk) lose the most mass at low burn temperatures (<300 ∘C), whereas heathland shrub leaves, brown moss, and ferns lose the most mass at high burn temperatures. This suggests that species with low mass retention in high-temperature fires are likely to be under-represented in the fossil charcoal record. The charcoal particle aspect ratio appeared to be the strongest indicator of the fuel type burnt. Graminoid charcoal particles are the most elongate (6.7–11.5), with a threshold above 6 that may be indicative of wetland graminoids; leaves are the shortest and bulkiest (2.1–3.5); and twigs and wood are intermediate (2.0–5.2). Further, the use of fine diagnostic features was more successful in separating wood, graminoids, and leaves, but it was difficult to further differentiate these fuel types due to overlapping features. High-aspect-ratio particles, dominated by graminoid and Sphagnum morphologies, may be robust indicators of low-temperature surface fires, whereas abundant wood and leaf morphologies as well as low-aspect-ratio particles are indicative of higher-temperature fires. However, the overlapping morphologies of leaves and wood from trees and shrubs make it hard to distinguish between high-intensity surface fires, combusting living shrubs and dead wood and leaves, and high-intensity crown fires that have burnt living trees. Distinct particle shape may also influence charcoal transportation, with elongated particles (graminoids) potentially having a more heterogeneous distribution and being deposited farther away from the origin of fire than the rounder, polygonal leaf particles. Despite these limitations, the combined use of charred-particle aspect ratios and fuel morphotypes can aid in the more robust interpretation of fuel source and fire-type changes. Lastly, I highlight the further investigations needed to refine the histories of past wildfires.
Deformation in the upper mantle is localized in shear zones. In order to localize strain, weakening has to occur, which can be achieved by a reduction in grain size. In order for grains to remain small and preserve shear zones, phases have to mix. Phase mixing leads to dragging or pinning of grain boundaries which slows down or halts grain growth. Multiple phase mixing processes have been suggested to be important during shear zone evolution. The importance of a phase mixing process depends on the geodynamic setting. This study presents detailed microstructural analysis of spinel bearing shear zones from the Erro-Tobbio peridotite (Italy) that formed during pre-alpine rifting. The first stage of deformation occurred under melt-free conditions, during which clinopyroxene and olivine porphyroclasts dynamically recrystallized. With ongoing extension, silica-undersaturated melt percolated through the shear zones and reacted with the clinopyroxene neoblasts, forming olivine–clinopyroxene layers. Furthermore, the melt reacted with orthopyroxene porphyroclasts, forming fine-grained polymineralic layers (ultramylonites) adjacent to the porphyroclasts. Strain rates in these layers are estimated to be about an order of magnitude faster than within the olivine-rich matrix. This study demonstrates the importance of melt-rock reactions for grain size reduction, phase mixing and strain localization in these shear zones.
With the Earth system being about to leave Holocene conditions and thus the known safe operating space for humanity, frameworks such as the Planetary Boundaries (PBs) and the Sustainable Development Goals (SDGs) provide quantitative metrics to guide sustainability transformations. In order to strive, not only for compliance with the PBs but also for societal well-being, some approaches attempt to combine both PBs and SDGs within a single assessment. We focus on two prominent examples, the “Doughnut” by Kate Raworth and the #SDGinPB project of the 2018 report to the Club of Rome, which are not only aimed at public outreach, but also at guiding policy-making. To meet these objectives, the approaches should possess a certain accuracy in determining the progress in achieving the SDGs and in complying with the PBs. We evaluate, by using a multi-indicator approach for comparison, whether both approaches’ limited set of indicators can still represent the SDGs’ complexity. This comparative approach estimates the progress in achieving SDGs, especially in the Global North, to be significantly lower. Based on these results and against the approaches’ purposes, we discuss their simplifications and at which point the results are no longer reliable. We conclude that global assessments can be an important factor in initiating transformative processes by stimulating public discourse, but that the actual implementation of these would require approaches with greater recognition of local particularities.
We combine structural analysis of fractures with 22 U–Pb dates measured in fracture-filling carbonate cements from bed-parallel fibrous calcite veins (beef), conjugated veins and faults within the Vaca Muerta Formation along the Andean fold and thrust belt in the Neuquén Basin. The measured ages constrain accurately the relationships between overpressures caused by hydrocarbon generation and Andean compression as mechanisms for natural fracturing and vein formation. Two generations of fibres have been identified in beef. The first one, consists of dark fibres from the inner zones, which are perpendicular to bedding and contain abundant cone-in-cone structures and hydrocarbon inclusions. U–Pb dating of these fibres yielded Early to Late Cretaceous ages from 116.7 ± 17.7 to 78.8 ± 10.2 Ma. The second generation of fibres corresponds to the outer zones and consists of white fibres oblique to bedding, indicating growth during layer-parallel shortening. Bed-perpendicular veins cutting beef yielded Late Cretaceous-late Palaeocene dates from 72.8 ± 22.4 to 60.9 ± 10.4 Ma. Eocene ages from 52.0 ± 2.9 to 42.2 ± 18.9 Ma were measured in bed-parallel slip surfaces and reverse and strike-slip faults, whereas Miocene dates from 13.9 ± 2.6 to 6.2 ± 1.1 Ma were measured in E-W calcite veins. U–Pb dating of veins, structural analysis of fractures and subsidence curves, indicate that beef inner zones formed in the oil window during burial of the Neuquén basin, and that tectonic stresses could enhance their formation. Beef outer zones and bed-perpendicular veins formed during E-W Late Cretaceous-late Palaeocene layer-parallel shortening. Contrarily, late Palaeocene-late Eocene bed-parallel slip surfaces and faults and Miocene E-W veins formed during NE-SW and E-W syn-to post-folding deformation, respectively. In both cases, syn-to post-folding compression occurred synchronously with forelandward migration of magmatic activity attributed to flat subduction of the Pacific slab beneath the Andes.
Aquatic ecosystems are globally contaminated with microplastics (MP). However, comparative data on MP levels in freshwater systems is still scarce. Therefore, the aim of this study is to quantify MP abundance in water and sediment of the German river Elbe using visual, spectroscopic (Fourier-transform infrared spectroscopy) and thermo analytical (pyrolysis gas chromatography mass spectrometry) methods. Samples from eleven German sites along the German part of the Elbe were collected, both in the water and sediment phase, in order to better understand MP sinks and transport mechanisms. MP concentrations differed between the water and sediment phase. Sediment concentrations (mean: 3,350,000 particles m−3, 125–5000 μm MP) were in average 600,000-fold higher than water concentrations (mean: 5.57 particles m−3, 150–5000 μm MP). The abundance varied between the sampling sites: In sediments, the abundance decreased in the course of the river while in water samples no such clear trend was observed. This may be explained by a barrage retaining sediments and limiting tidal influence in the upstream parts of the river. Particle shape differed site-specifically with one site having exceptionally high quantities of spheres, most probably due to industrial emissions of PS-DVB resin beads. Suspended MP consisted predominantly of polyethylene and polypropylene whereas sediments contained a higher diversity of polymer types. Determined MP concentrations correspond well to previous results from other European rivers. In a global context, MP levels in the Elbe relate to the lower (water) to middle section (sediment) of the global range of MP concentrations determined for rivers worldwide. This highlights that elevated MP levels are not only found in single countries or continents, but that MP pollution is an issue of global concern.
Motions on planetary spatial scales in the atmosphere are governed by the planetary geostrophic equations. However, little attention has been paid to the interaction between the baroclinic and barotropic flows within the planetary geostrophic scaling. This is the focus of the present study, which utilizes planetary geostrophic equations for a Boussinesq fluid supplemented by a novel evolution equation for the barotropic flow. The latter is affected by meridional momentum flux due to baroclinic flow and drag by the surface wind. The barotropic wind, on the other hand, affects the baroclinic flow through buoyancy advection. Via a relaxation towards a prescribed buoyancy profile the model produces realistic major features of the zonally symmetric wind and temperature fields. We show that there is considerable cancellation between the barotropic and the baroclinic surface zonal mean zonal winds. Linear and nonlinear model responses to steady diabatic zonally asymmetric forcing are investigated, and the arising stationary waves are interpreted in terms of analytical solutions. We also study the problem of baroclinic instability on the sphere within the present model.
Chondrules are thought to play a crucial role in planet formation, but the mechanisms leading to their formation are still a matter of unresolved discussion. So far, experiments designed to understand chondrule formation conditions have been carried out only under the influence of terrestrial gravity. In order to introduce more realistic conditions, we developed a chondrule formation experiment, which was carried out at long-term microgravity aboard the International Space Station. In this experiment, freely levitating forsterite (Mg2SiO4) dust particles were exposed to electric arc discharges, thus simulating chondrule formation via nebular lightning. The arc discharges were able to melt single dust particles completely, which then crystallized with very high cooling rates of >105 K h−1. The crystals in the spherules show a crystallographic preferred orientation of the [010] axes perpendicular to the spherule surface, similar to the preferred orientation observed in some natural chondrules. This microstructure is probably the result of crystallization under microgravity conditions. Furthermore, the spherules interacted with the surrounding gas during crystallization. We show that this type of experiment is able to form spherules, which show some similarities with the morphology of chondrules despite very short heating pulses and high cooling rates.
A massive occurrence of microbial carbonates, including abundant sponge remains, within the Devonian Elbingerode Reef Complex was likely deposited in a former cavity of the fore-reef slope during the early Frasnian. It is suggested that the formation of microbial carbonate was to a large part favored by the activity of heterotrophic, i.e., sulfate-reducing bacteria, in analogy to Quaternary coral reef microbialites. The Elbingerode Reef Complex is an example of an oceanic or Darwinian barrier reef system. In modern barrier reef settings, microbialite formation is commonly further facilitated by weathering products from the central volcanic islands. The Devonian microbialites of the Elbingerode Reef Complex occur in the form of reticulate and laminated frameworks. Reticulate framework is rich in hexactinellid glass sponges, the tissue decay of which led to the formation of abundant micrite as well as peloidal and stromatactis textures. Supposed calcimicrobes such as Angusticellularia (formerly Angulocellularia) and Frutexites, also known from cryptic habitats, were part of the microbial association. The microbial degradation of sponge tissue likely also contributed to the laminated framework accretion as evidenced by the occurrence of remains of so-called “keratose” demosponges. Further typical textures in the microbialite of the Elbingerode Reef Complex include zebra limestone, i.e., the more or less regular intercalation of microbial carbonate and cement. Elevated concentrations of magnesium in the microbialite as compared to the surrounding metazoan (stromatoporoid-coral) reef limestone suggests that the microbialite of the Elbingerode Reef Complex was initially rich in high-magnesium calcite, which would be yet another parallel to modern, cryptic coral reef microbial carbonates. Deposition and accretion of the microbialite largely occurred in oxygenated seawater with suboxic episodes as indicated by the trace element (REE + Y) data.
Motivated by the question of whether and how wave–wave interactions should be implemented into atmospheric gravity-wave parametrizations, the modulation of triadic gravity-wave interactions by a slowly varying and vertically sheared mean flow is considered for a non-rotating Boussinesq fluid with constant stratification. An analysis using a multiple-scale WKBJ (Wentzel–Kramers–Brillouin–Jeffreys) expansion identifies two distinct scaling regimes, a linear off-resonance regime, and a nonlinear near-resonance regime. Simplifying the near-resonance interaction equations allows for the construction of a parametrization for the triadic energy exchange which has been implemented into a one-dimensional WKBJ ray-tracing code. Theory and numerical implementation are validated for test cases where two wave trains generate a third wave train while spectrally passing through resonance. In various settings, of interacting vertical wavenumbers, mean-flow shear, and initial wave amplitudes, the WKBJ simulations are generally in good agreement with wave-resolving simulations. Both stronger mean-flow shear and smaller wave amplitudes suppress the energy exchange among a resonantly interacting triad. Experiments with mean-flow shear as strong as in the vicinity of atmospheric jets suggest that internal gravity-wave dynamics are dominated in such regions by wave modulation. However, triadic gravity-wave interactions are likely to be relevant in weakly sheared regions of the atmosphere.
Triple oxygen isotope measurements are an emerging tool in paleoclimate reconstructions. In this contribution we develop the application of triple oxygen isotope measurements to lacustrine sediments to reconstruct past elevations. We focus on a well-constrained sample set from the Eocene North American Cordillera (Cherty Limestone Formation, Elko Basin, NV, United States, 42–43.5 Ma) on the east side of the elevated Nevadaplano. We present triple oxygen isotope measurements on freshwater lacustrine chert samples from the Cherty Limestone Formation. Across an evaporation trend spanning 6.5‰ in δ18O values we observe a negative correlation with Δ′17O ranging from −0.066 to −0.111‰ (λRL = 0.528), with an empirical slope (λchert, δ′17O vs. δ′18O) of 0.5236. Additionally, we present new carbonate clumped isotope (Δ47) temperature results on the overlying fluvial-lacustrine Elko Formation, which indicate an error-weighted mean temperature of 32.5 ± 3.8°C (1σ), and evaporatively enriched lake water spanning δ18O values of −3.7 to +3.5‰ (VSMOW). Paired chert and carbonate δ18O values demonstrate that co-equilbrium among the carbonate and chert phases is unlikely. Thus, as also previously suggested, it is most likely that Elko Basin chert formed during early diagenesis in equilbirium with pore waters that reflect evaporatively 18O-enriched lake water. Using this scenario we apply a model for back-calculating unevaporated water composition to derive a source water of δ′18O = −16.1‰ (VSMOW), similar to modern local meteoric waters but lower than previous work on paired δ18O- δD measurements from the same chert samples. Further, this back-calculated unevaporated source water is higher than those derived using δD measurements of Late Eocene hydrated volcanic glass from the Elko Basin (average δ′18O equivalent of approximately −18.4‰, VSMOW). This suggests, assuming Eocene meteoric water Δ′17O values similar to today (∼0.032‰), either that: (1) the hypsometric mean elevation recorded by the lacustrine Cherty Limestone was lower than that derived from the average of the volcanic glass δD measurements alone; or (2) there was hydrogen exchange in volcanic glass with later low δD meteoric fluids. Nonetheless, our new findings support a relatively high (∼2.5–3 km) plateau recorded in the Elko Basin during the mid-Eocene.
Drought is understood as both a lack of water (i.e., a deficit compared to demand) and a temporal anomaly in one or more components of the hydrological cycle. Most drought indices, however, only consider the anomaly aspect, i.e., how unusual the condition is. In this paper, we present two drought hazard indices that reflect both the deficit and anomaly aspects. The soil moisture deficit anomaly index, SMDAI, is based on the drought severity index, DSI (Cammalleri et al., 2016), but is computed in a more straightforward way that does not require the definition of a mapping function. We propose a new indicator of drought hazard for water supply from rivers, the streamflow deficit anomaly index, QDAI, which takes into account the surface water demand of humans and freshwater biota. Both indices are computed and analyzed at the global scale, with a spatial resolution of roughly 50 km, for the period 1981–2010, using monthly time series of variables computed by the global water resources and the model WaterGAP 2.2d. We found that the SMDAI and QDAI values are broadly similar to values of purely anomaly-based indices. However, the deficit anomaly indices provide more differentiated spatial and temporal patterns that help to distinguish the degree and nature of the actual drought hazard to vegetation health or the water supply. QDAI can be made relevant for stakeholders with different perceptions about the importance of ecosystem protection, by adapting the approach for computing the amount of water that is required to remain in the river for the well-being of the river ecosystem. Both deficit anomaly indices are well suited for inclusion in local or global drought risk studies.
Analysing the composition of ambient ultrafine particles (UFPs) is a challenging task due to the low mass and chemical complexity of small particles, yet it is a prerequisite for the identification of particle sources and the assessment of potential health risks. Here, we show the molecular characterization of UFPs, based on cascade impactor (Nano-MOUDI) samples that were collected at an air quality monitoring station near one of Europe's largest airports, in Frankfurt, Germany. At this station, particle-size-distribution measurements show an enhanced number concentration of particles smaller than 50 nm during airport operating hours. We sampled the lower UFP fraction (0.010–0.018, 0.018–0.032, 0.032–0.056 µm) when the air masses arrived from the airport. We developed an optimized filter extraction procedure using ultra-high-performance liquid chromatography (UHPLC) for compound separation and a heated electrospray ionization (HESI) source with an Orbitrap high-resolution mass spectrometer (HRMS) as a detector for organic compounds. A non-target screening detected ∼200 organic compounds in the UFP fraction with sample-to-blank ratios larger than 5. We identified the largest signals as homologous series of pentaerythritol esters (PEEs) and trimethylolpropane esters (TMPEs), which are base stocks of aircraft lubrication oils. We unambiguously attribute the majority of detected compounds to jet engine lubrication oils by matching retention times, high-resolution and accurate mass measurements, and comparing tandem mass spectrometry (MS2) fragmentation patterns between both ambient samples and commercially available jet oils. For each UFP stage, we created molecular fingerprints to visualize the complex chemical composition of the organic fraction and their average carbon oxidation state. These graphs underline the presence of the homologous series of PEEs and TMPEs and the appearance of jet oil additives (e.g. tricresyl phosphate, TCP). Targeted screening of TCP confirmed the absence of the harmful tri-ortho isomer, while we identified a thermal transformation product of TMPE-based lubrication oil (trimethylolpropane phosphate, TMP-P). Even though a quantitative determination of the identified compounds is limited, the presented method enables the qualitative detection of molecular markers for jet engine lubricants in UFPs and thus strongly improves the source apportionment of UFPs near airports.
Drought is understood as both a lack of water (i.e., a deficit as compared to some requirement) and an anomaly in the condition of one or more components of the hydrological cycle. Most drought indices, however, only consider the anomaly aspect, i.e., how unusual the condition is. In this paper, we present two drought hazard indices that reflect both the deficit and anomaly aspects. The soil moisture deficit anomaly index, SMDAI, is based on the drought severity index, DSI, but is computed in a more straightforward way that does not require the definition of a mapping function. We propose a new indicator of drought hazard for water supply from rivers, the streamflow deficit anomaly index, QDAI, which takes into account the surface water demand of humans and freshwater biota. Both indices are computed and analyzed at the global scale, with a spatial resolution of roughly 50 km, for the period 1981-2010, using monthly time series of variables computed by the global water resources and the model WaterGAP2.2d. We found that the SMDAI and QDAI values are broadly similar to values of purely anomaly-based indices. However, the deficit anomaly indices provide more differentiated, spatial and temporal patterns that help to distinguish the degree of the actual drought hazard to vegetation health or the water supply. QDAI can be made relevant for stakeholders with different perceptions about the importance of ecosystem protection, by adapting the approach for computing the amount of water that is required to remain in the river for the well being of the river ecosystem. Both deficit anomaly indices are well suited for inclusion in local or global drought risk studies.
Analysing the composition of ambient ultrafine particles (UFP) is a challenging task due to the low mass and chemical complexity of small particles, yet it is a prerequisite for the identification ofparticle sources and the assessment of potential health risks. Here, we show the molecular characterization of UFP, based on cascade impactor (Nano-MOUDI) 10samples that were collected at an air quality monitoring station nearby one of Europe`s largest airports in Frankfurt, Germany. At this station, particle-size-distribution measurements show enhanced number concentration of particles smaller than 50nm during airport operating hours. We sampled the lower UFP fraction (0.010-0.018 μm; 0.018-0.032 μm; 0.032-0.056 μm) when the air masses arrived from the airport. We developed an optimized filter extraction procedure, used ultra-high performance liquid chromatography (UHPLC) for compound separation, and a heated electrospray ionization (HESI) source with an 15Orbitrap high-resolution mass spectrometer (HRMS) as a detector for organic compounds. A non-target screening detected ~200 organic compounds in the UFP fraction with sample-to-blank ratios larger than five. We identified the largest signals as homologous series of pentaerythritol esters (PEE) and trimethylolpropane esters (TMPE), which are base stocks of aircraft lubrication oils. We unambiguously attribute the majority of detected compounds to jet engine lubrication oils by matching retention times, high-resolution/accurate mass (HR/AM) measurements, and comparing MS/MS fragmentation patterns between both ambient samples and commercially available jet oils. For each UFP stage, we created molecular fingerprints to visualize the complex chemical composition ofthe organic fraction and their average carbon oxidation state. These graphs underline the presence of the homologous series of PEE and TMPE, and the appearance of jet oil additives (e.g. tricresyl phosphate (TCP)). Targeted screening on TCP confirmed the absence of the harmful tri-orthoisomer, while we identified a thermal transformation product of TMPE-based lubrication oil (trimethylolpropane phosphate (TMP-P)). Even though a quantitative determination of the identified compounds is limited, the presented method enables the qualitative detection of molecular markers for jet engine lubricants in UFP and thus strongly improves the source apportionment of UFP near airports.