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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.
Measurement of iodine species and sulfuric acid using bromide chemical ionization mass spectrometers
(2021)
Iodine species are important in the marine atmosphere for oxidation and new-particle formation. Understanding iodine chemistry and iodine new-particle formation requires high time resolution, high sensitivity, and simultaneous measurements of many iodine species. Here, we describe the application of a bromide chemical ionization mass spectrometer (Br-CIMS) to this task. During the iodine oxidation experiments in the Cosmics Leaving OUtdoor Droplets (CLOUD) chamber, we have measured gas-phase iodine species and sulfuric acid using two Br-CIMS, one coupled to a Multi-scheme chemical IONization inlet (Br-MION-CIMS) and the other to a Filter Inlet for Gasses and AEROsols inlet (Br-FIGAERO-CIMS). From offline calibrations and intercomparisons with other instruments, we have quantified the sensitivities of the Br-MION-CIMS to HOI, I2, and H2SO4 and obtained detection limits of 5.8 × 106, 3.8 × 105, and 2.0 × 105 molec. cm−3, respectively, for a 2 min integration time. From binding energy calculations, we estimate the detection limit for HIO3 to be 1.2 × 105 molec. cm−3, based on an assumption of maximum sensitivity. Detection limits in the Br-FIGAERO-CIMS are around 1 order of magnitude higher than those in the Br-MION-CIMS; for example, the detection limits for HOI and HIO3 are 3.3 × 107 and 5.1 × 106 molec. cm−3, respectively. Our comparisons of the performance of the MION inlet and the FIGAERO inlet show that bromide chemical ionization mass spectrometers using either atmospheric pressure or reduced pressure interfaces are well-matched to measuring iodine species and sulfuric acid in marine environments.
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.
Droughts are anticipated to intensify in many parts of the world due to climate change. However, the issue of drought definition, namely the diversity of drought indices, makes it difficult to compare drought assessments. This issue is widely known, but its relative importance has never been quantitatively evaluated in comparison to other sources of uncertainty. Here, encompassing three drought categories (meteorological, agricultural, and hydrological droughts) with four temporal scales of interest, we evaluated changes in the drought frequency using multi-model and multi-scenario simulations to identify areas where the definition issue could result in pronounced uncertainties and to what extent. We investigated the disagreement in the signs of changes between drought definitions and decomposed the variance into four main factors: drought definitions, greenhouse gas concentration scenarios, global climate models, and global water models, as well as their interactions. The results show that models were the primary sources of variance over 82% of the global land area. On the other hand, the drought definition was the dominant source of variance in the remaining 17%, especially in parts of northern high-latitudes. Our results highlight specific regions where differences in drought definitions result in a large spread among projections, including areas showing opposite signs of significant changes. At a global scale, 7% of the variance resulted independently from the definition issue, and that value increased to 44% when 1st and 2nd order interactions were considered. The quantitative results suggest that by clarifying hydrological processes or sectors of interest, one could avoid these uncertainties in drought assessments to obtain a clearer picture of future drought change.
A general circulation model is used to study the interaction between parameterized gravity waves (GWs) and large-scale Kelvin waves in the tropical stratosphere. The simulation shows that Kelvin waves with substantial amplitudes (∼10 m s−1) can significantly affect the distribution of GW drag by modulating the local shear. Furthermore, this effect is localized to regions above strong convective organizations that generate large-amplitude GWs, so that at a given altitude it occurs selectively in a certain phase of Kelvin waves. Accordingly, this effect also contributes to the zonal-mean GW drag, which is large in the middle stratosphere during the phase transition of the quasi-biennial oscillation (QBO). Furthermore, we detect an enhancement of Kelvin-wave momentum flux due to GW drag modulated by Kelvin waves. The result implies an importance of GW dynamics coupled to Kelvin waves in the QBO progression.
Plain Language Summary: The variability of the tropical atmosphere at altitudes of about 18–40 km is dominated by a large-amplitude long-term oscillation of wind, the quasi-biennial oscillation, which has a broad impact on the climate and seasonal forecasting. This oscillation is known to be driven by various types of atmospheric waves with multiple spatial scales. Using a numerical model, this study reports a process of interaction between those waves on different scales, which has not been illuminated before. The result implies a potential importance of this process in the progression of the quasi-biennial oscillation. Proper model representations of these multiscale waves and tropical convection are required to simulate this process.
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.
The Global South is facing severe challenges in ensuring livelihood security due to climate change impacts, environmental degradation and population growth as well as changing lifestyles. These complex problems cannot be solely solved by single scientific disciplines – they require transdisciplinary research (TDR). Stakeholders from civil society, the corporate sector, government and science need to pool their knowledge to find solutions for sustainable transformations. In Namibia, we have been involved in TDR projects on water supply, and sanitation services as well as livestock management in rangeland systems. In this paper, we review two TDR projects that differ in multiple ways and hence allow us to carve out structural differences and critically discuss research outcomes, lessons learned and the challenge of North–South collaborations. Our review builds upon published and unpublished project documents as well as expert interviews with Namibian and German researchers who were involved in the projects. Our results show that TDR can be put into practice in different ways, depending on the research focus and the period available. The TDR phases of problem framing, inter- and transdisciplinary integration were implemented with different tools and foci points. We discuss the role of project length and funding conditions for project success and outcome generation. In addition, we critically consider the role of Namibian and German researchers in these international collaborations. The conclusions we draw touch upon the points of preparatory research funding, the equal acknowledgement of Global South contributions to joint research projects and the explicit handling of TDR components in project work. Significance: • The current social-ecological challenges are complex and require TDR as a mode of knowledge coproduction, particularly in a development context. • Inter- and transdisciplinary integration are critical processes for a project to be successful and require the allocation of adequate time and monetary resources. • Longer-term projects with a funded preparatory research phase constitute a structural model for TDR as project outcomes can evolve over time. • Global South researchers carry a hidden burden in international collaborations that has to be adequately acknowledged upfront in project planning and final products.
Biogenic organic precursors play an important role in atmospheric new particle formation (NPF). One of the major precursor species is α-pinene, which upon oxidation can form a suite of products covering a wide range of volatilities. Highly oxygenated organic molecules (HOMs) comprise a fraction of the oxidation products formed. While it is known that HOMs contribute to secondary organic aerosol (SOA) formation, including NPF, they have not been well studied in newly formed particles due to their very low mass concentrations. Here we present gas- and particle-phase chemical composition data from experimental studies of α-pinene oxidation, including in the presence of isoprene, at temperatures (−50 and −30 ∘C) and relative humidities (20 % and 60 %) relevant in the upper free troposphere. The measurements took place at the CERN Cosmics Leaving Outdoor Droplets (CLOUD) chamber. The particle chemical composition was analyzed by a thermal desorption differential mobility analyzer (TD-DMA) coupled to a nitrate chemical ionization–atmospheric pressure interface–time-of-flight (CI-APi-TOF) mass spectrometer. CI-APi-TOF was used for particle- and gas-phase measurements, applying the same ionization and detection scheme. Our measurements revealed the presence of C8−10 monomers and C18−20 dimers as the major compounds in the particles (diameter up to ∼ 100 nm). Particularly, for the system with isoprene added, C5 (C5H10O5−7) and C15 compounds (C15H24O5−10) were detected. This observation is consistent with the previously observed formation of such compounds in the gas phase. However, although the C5 and C15 compounds do not easily nucleate, our measurements indicate that they can still contribute to the particle growth at free tropospheric conditions. For the experiments reported here, most likely isoprene oxidation products enhance the growth of particles larger than 15 nm. Additionally, we report on the nucleation rates measured at 1.7 nm (J1.7 nm) and compared with previous studies, we found lower J1.7 nm values, very likely due to the higher α-pinene and ozone mixing ratios used in the present study.
Biogenic organic precursors play an important role in atmospheric new particle formation (NPF). One of the major precursor species is α-pinene, which upon oxidation can form a suite of products covering a wide range of volatilities. Highly oxygenated organic molecules (HOMs) comprise a fraction of the oxidation products formed. While it is known that HOMs contribute to secondary organic aerosol (SOA) formation, including NPF, they have not been well studied in newly formed particles due to their very low mass concentrations. Here we present gas- and particle-phase chemical composition data from experimental studies of α-pinene oxidation, including in the presence of isoprene, at temperatures (−50 and −30 ∘C) and relative humidities (20 % and 60 %) relevant in the upper free troposphere. The measurements took place at the CERN Cosmics Leaving Outdoor Droplets (CLOUD) chamber. The particle chemical composition was analyzed by a thermal desorption differential mobility analyzer (TD-DMA) coupled to a nitrate chemical ionization–atmospheric pressure interface–time-of-flight (CI-APi-TOF) mass spectrometer. CI-APi-TOF was used for particle- and gas-phase measurements, applying the same ionization and detection scheme. Our measurements revealed the presence of C8−10 monomers and C18−20 dimers as the major compounds in the particles (diameter up to ∼ 100 nm). Particularly, for the system with isoprene added, C5 (C5H10O5−7) and C15 compounds (C15H24O5−10) were detected. This observation is consistent with the previously observed formation of such compounds in the gas phase. However, although the C5 and C15 compounds do not easily nucleate, our measurements indicate that they can still contribute to the particle growth at free tropospheric conditions. For the experiments reported here, most likely isoprene oxidation products enhance the growth of particles larger than 15 nm. Additionally, we report on the nucleation rates measured at 1.7 nm (J1.7 nm) and compared with previous studies, we found lower J1.7 nm values, very likely due to the higher α-pinene and ozone mixing ratios used in the present study.
At high pressures, autoionization – along with polymerization and metallization – is one of the responses of simple molecular systems to a rise in electron density. Nitrosonium nitrate (NO+NO3−), known for this property, has attracted a large interest in recent decades and was reported to be synthesized at high pressure and high temperature from a variety of nitrogen–oxygen precursors, such as N2O4, N2O and N2–O2 mixtures. However, its structure has not been determined unambiguously. Here, we present the first structure solution and refinement for nitrosonium nitrate on the basis of single-crystal X-ray diffraction at 7.0 and 37.0 GPa. The structure model (P21/m space group) contains the triple-bonded NO+ cation and the NO3− sp2-trigonal planar anion. Remarkably, crystal-chemical considerations and accompanying density-functional-theory calculations show that the oxygen atom of the NO+ unit is positively charged – a rare occurrence when in the presence of a less-electronegative element.