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Nontarget screening exhibits a seasonal cycle of PM2.5 organic aerosol composition in Beijing
(2022)
Ma, Jialiang ; Ungeheuer, Florian ; Zheng, Feixue ; Du, Wei ; Wang, Yonghong ; Cai, Jing ; Zhou, Ying ; Yan, Chao ; Liu, Yongchun ; Kulmala, Markku ; Daellenbach, Kaspar Rudolf ; Vogel, Alexander L.
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.
Wallraff, Jonas Peter ; Ungeheuer, Florian ; Dombrowski, Andrea ; Oehlmann, Jörg ; Vogel, Alexander L.
This study describes the chemical composition and in vitro toxicity of the organic fraction of fine particulate matter (PM2.5) at an urban background site, which receives emissions either from Frankfurt international airport or the city centre, respectively. We analysed the chemical composition of filter extracts (PM2.5) using ultrahigh-performance liquid chromatography coupled to a high-resolution mass spectrometer, followed by a non-target analysis. In parallel, we applied the bulk of the filter extracts to a Microtox and acetylcholinesterase-inhibition assay for in vitro toxicity testing. We find that both the chemical composition and toxicity depend on the prevailing wind directions, and the airport operating condition, respectively. The occurrence of the airport marker compounds tricresyl phosphate and pentaerythritol esters depends on the time of the day, reflecting the night flight ban as well as an airport strike event during November 2019. We compared the organic aerosol composition and toxicity from the airport wind-sector against the city centre wind-sector. We find that urban background aerosol shows a higher baseline toxicity and acetylcholinesterase inhibition compared to rural PM2.5 that is advected over the airport. Our results indicate that the concentration and individual composition of PM2.5 influence the toxicity. Suspected drivers of the acetylcholinesterase inhibition are i.e. organophosphorus esters like triphenyl phosphate and cresyldiphenyl phosphate, and the non-ionic surfactant 4-tert-octylphenol ethoxylate. However, further research is necessary to unambiguously identify harmful organic air pollutants and their sources and quantify concentration levels at which adverse effects in humans and the environment can occur.
Nucleation of jet engine oil vapours is a large source of aviation-related ultrafine particles
(2022)
Ungeheuer, Florian ; Caudillo, Lucía ; Ditas, Florian ; Simon, Mario ; Pinxteren, Dominik van ; Kılıç, Doğuşhan ; Rose, Diana ; Jacobi, Stefan ; Kürten, Christoph Andreas ; Curtius, Joachim ; Vogel, Alexander L.
Large airports are a major source of ultrafine particles, which spread across densely populated residential areas, affecting air quality and human health. Jet engine lubrication oils are detectable in aviation-related ultrafine particles, however, their role in particle formation and growth remains unclear. Here we show the volatility and new-particle-formation ability of a common synthetic jet oil, and the quantified oil fraction in ambient ultrafine particles downwind of Frankfurt International Airport, Germany. We find that the oil mass fraction is largest in the smallest particles (10-18 nm) with 21% on average. Combining ambient particle-phase concentration and volatility of the jet oil compounds, we determine a lower-limit saturation ratio larger than 1 × 105 for ultra-low volatility organic compounds. This indicates that the oil is an efficient nucleation agent. Our results demonstrate that jet oil nucleation is an important mechanism that can explain the abundant observations of high number concentrations of non-refractory ultrafine particles near airports.
Li6UO6 has a reversible phase transformation at 680°C and decomposes above about 850°C. At high pressure the low temperature modification becomes unstable because of an invariant point in the system Li2O—Li4UO5 at approximately 13 Kb and 620°C. β-Li6UO6 has a triclinic unit cell with a = 5.203, b= 5.520, c = 5.536 Å, α = 114.7, β = 120.7 and γ = 75.5°. The close relationship between the crystal structures of Li6TeO6 and Li6UO6 is also suggested from similar infrared spectra and from partial solid solution Li6UO6—Li6TeO6.
Airborne transmission of SARS-CoV-2 through virus-containing aerosol particles has been established as an important pathway for Covid-19 infection. Suitable measures to prevent such infections are imperative, especially in situations when a high number of persons convene in closed rooms. Here we tested the efficiency and practicability of operating four air purifiers equipped with HEPA filters in a high school classroom while regular classes were taking place. We monitored the aerosol number concentration for particles > 3 nm at two locations in the room, the aerosol size distribution in the range from 10 nm to 10 µm, PM10 and CO2 concentration. For comparison, we performed similar measurements in a neighboring classroom without purifiers. In times when classes were conducted with windows and door closed, the aerosol concentration was reduced by more than 90 % within less than 30 minutes when running the purifiers (air exchange rate 5.5 h-1). The reduction was homogeneous throughout the room and for all particle sizes. The measurements are supplemented by a calculation estimating the maximum concentration levels of virus-containing aerosol from a highly contagious person speaking in a closed room with and without air purifiers. Measurements and calculation demonstrate that air purifiers potentially represent a well-suited measure to reduce the risks of airborne transmission of SARS-CoV-2 substantially. Staying for two hours in a closed room with a highly infective person, we estimate that the inhaled dose is reduced by a factor of six when using air purifiers with a total air exchange rate of 5.7 h-1.
Airborne transmission of SARS-CoV-2 through virus-containing aerosol particles has been established as an important pathway for Covid-19 infection. Suitable measures to prevent such infections are imperative, especially in situations when a high number of persons convene in closed rooms. Here we tested the efficiency and practicability of operating four air purifiers equipped with HEPA filters in a high school classroom while regular classes were taking place. We monitored the aerosol number concentration for particles >3 nm at two locations in the room, the aerosol size distribution in the range from 10 nm to 10 µm, PM10 and CO2 concentration. For comparison, we performed similar measurements in a neighboring classroom without purifiers. In times when classes were conducted with windows and door closed, the aerosol concentration was reduced by more than 90% within less than 30 min when running the purifiers (air exchange rate 5.5 h−1). The reduction was homogeneous throughout the room and for all particle sizes. The measurements are supplemented by a calculation estimating the maximum concentration levels of virus-containing aerosol from a highly contagious person speaking in a closed room with and without air purifiers. Measurements and calculation demonstrate that air purifiers potentially represent a well-suited measure to reduce the risks of airborne transmission of SARS-CoV-2 substantially. Staying for 2 h in a closed room with a highly infective person, we estimate that the inhaled dose is reduced by a factor of six when using air purifiers with a total air exchange rate of 5.7 h−1.
WaterGAP (Water - Global Assessment and Prognosis) is a tool for modeling global water use and water availability. It participates among other models in the ISIMIP initiative (The Inter-Sectoral Impact Model Intercomparison Project). As part of this initiative, the water temperature should be calculated by participating hydrological models because it plays a vital role in many chemical, physical and biological processes. Therefore, the subject of this master thesis is to implement the physically based surface water temperature computation after VAN BEEK ET AL. (2012) and WANDERS ET AL. (2019) into WaterGAP and compare the results to the statistical regression approach by PUNZET ET AL. (2012). The computation is validated with observed water temperature data obtained from the GEMStat water quality database. The results are good for arctic and temperate latitudes. Surface water temperatures for tropical rivers are overestimated, most likely due to the overestimation of precipitation temperatures, incoming radiation and groundwater temperatures. The comparison with the regression model by PUNZET ET AL. (2012) shows matching results. The regression model even matches with WaterGAP results for most of the simulations of the future under climate change conditions, where the regression model should stop working due to changing environmental parameters. Several assumptions had to be made in order to implement the water temperature calculation in Water-GAP. These include, e.g., discharge temperatures for power plant cooling water, precipitation and surface runoff temperatures. For model improvements, perhaps three different values for the different regions of the world should be used to cool down the precipitation and surface runoff. The model could also be improved by refining the ice formation calculation, especially for the conditions when the ice melts, breaks up and is transported downstream. Furthermore, the feedback to the river channel roughness could be implemented if ice has formed. The WaterGAP model upgraded with the water temperature calculation will help the ISIMIP initiative in the future.
The reanalysis products and derived products, ERA5 (Copernicus Climate Change Service, 2018) and W5E5 (WATCH Forcing Data (WFD) methodology applied to ERA5) (LANGE ET AL., 2021) have been recently published initiating a new phase of scientific research utilizing these datasets. ERA5 and W5E5 offer the possibility to reduce insecurities in model results through their improved quality compared to previous climate reanalyses (CUCCHI ET AL., 2020). The suitability of either climate forcing as input for the hydrological model WaterGAP and the influence of the models specific calibration routine has been evaluated with four model experiments. The model was validated by analysing the models ability to produce reasonable values for global water balance components and to reproduce observed discharge in 1427 basins as well as total water storage anomalies in 143 basins using well established efficiency metrics. Bias correction of W5E5 was found to lead to more global realistic mean precipitation and consequently discharge and AET values. In an uncalibrated model setup ERA5 results in better performances across all efficiency metrics. Model results produced with W5E5 as climate input were strongly improved through calibration ultimately leading to the best performances out of all four model experiments. However, model performances considerably improved through calibration with both climate forcings hence calibration was found to have the strongest effect on model performance. Furthermore, spatial differences in performance of either forcing were identified. Snow-dominated regions show an overall better performance with ERA5, while wetter and warmer regions are better represented with W5E5. Finally, it can be concluded that W5E5 should be preferred as climate input for impact modelling; however, depending on the spatial scale and region ERA5 should at least be considered, in particular for snow-dominated regions.
Unsichtbare Winzlinge
(2023)
Central Europe was affected by a compressional tectonic event in the Late Cretaceous, caused by the convergence of Iberia and Europe. Basement uplifts, inverted graben structures and newly formed marginal troughs are the main expressions of crustal shortening. Although the maximum activity occurred in a short period between 90 and 75 Ma, the exact timing of this event is still unclear. Dating of start and end of basin inversion is very different depending on the applied method. On the basis of borehole data, facies and thickness maps, the timing of basin re-organisation was reconstructed for several basins in Central Europe. The obtained data point to a synchronous start of basin inversion already at 95 Ma (Cenomanian), 5 Million years earlier than commonly assumed. The end of the Late Cretaceous compressional event is more difficult to pinpoint, because regional uplift and salt migration disturb the signal of shifting marginal troughs. Unconformities of Late Campanian to Paleogene age on inverted structures indicate slowly declining uplift rates.
Teleconnections of the Quasi-Biennial Oscillation in a multi-model ensemble of QBO-resolving models
(2021)
Anstey, James A. ; Simpson, Isla R. ; Richter, Jadwiga H. ; Naoe, Hiroaki ; Taguchi, Masakazu ; Serva, Federico ; Gray, Lesley J. ; Butchart, Neal ; Hamilton, Kevin ; Osprey, Scott ; Bellprat, Omar ; Braesicke, Peter ; Bushell, Andrew C. ; Cagnazzo, Chiara ; Chen, Chih-Chieh ; Chun, Hye-Yeong ; Garcia, Rolando R. ; Holt, Laura ; Kawatani, Yoshio ; Kerzenmacher, Tobias ; Kim, Young-Ha ; Lott, Francois ; McLandress, C. ; Scinocca, John ; Stockdale, Timothy N. ; Versick, Stefan ; Watanabe, Shingo ; Yoshida, Kohei ; Yukimoto, Seiji
The Quasi-biennial Oscillation (QBO) dominates the interannual variability of the tropical stratosphere and influences other regions of the atmosphere. The high predictability of the QBO implies that its teleconnections could lead to increased skill of seasonal and decadal forecasts provided the relevant mechanisms are accurately represented in models. Here modelling and sampling uncertainties of QBO teleconnections are examined using a multi-model ensemble of QBO-resolving atmospheric general circulation models that have carried out a set of coordinated experiments as part of the Stratosphere-troposphere Processes And their Role in Climate (SPARC) QBO initiative (QBOi). During Northern Hemisphere winter, the stratospheric polar vortex in most of these models strengthens when the QBO near 50 hPa is westerly and weakens when it is easterly, consistent with, but weaker than, the observed response. These weak responses are likely due to model errors, such as systematically weak QBO amplitudes near 50 hPa, affecting the teleconnection. The teleconnection to the North Atlantic Oscillation is less well captured overall, but of similar strength to the observed signal in the few models that do show it. The models do not show clear evidence of a QBO teleconnection to the Northern Hemisphere Pacific-sector subtropical jet.
Measurement of iodine species and sulfuric acid using bromide chemical ionization mass spectrometers
(2021)
Wang, Mingyi ; He, Xu-Cheng ; Finkenzeller, Henning ; Iyer, Siddharth ; Chen, Dexian ; Shen, Jiali ; Simon, Mario ; Hofbauer, Victoria ; Kirkby, Jasper ; Curtius, Joachim ; Maier, Norbert ; Kurtén, Theo ; Worsnop, Douglas R. ; Kulmala, Markku ; Rissanen, Matti P. ; Volkamer, Rainer ; Tham, Yee Jun ; Donahue, Neil McPherson ; Sipilä, Mikko
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.
Marinou, Eleni ; Amiridis, Vassilis ; Ansmann, Albert ; Nenes, Athanasios ; Balis, Dimitris ; Schrod, Jann Erik ; Binietoglou, Ioannis ; Solomos, Stavros ; Mamali, Dimitra ; Engelmann, Ronny ; Baars, Holger ; Kottas, Michael ; Tsekeri, Alexandra ; Proestakis, Emmanouil ; Kokkalis, Panagiotis ; Goloub, Philippe ; Cvetković, Bojan ; Nichovic, Slobodan ; Mamouri, Rodanthi ; Pikridas, Michael ; Stavroulas, Iasonas ; Keleshis, Christos ; Sciare, Jean
By means of available ice nucleating particle (INP) parameterization schemes we compute profiles of dust INP number concentration utilizing Polly-XT and CALIPSO lidar observations during the INUIT-BACCHUS-ACTRIS 2016 campaign. The polarization-lidar photometer networking (POLIPHON) method is used to separate dust and non-dust aerosol backscatter, extinction, mass concentration, particle number concentration (for particles with radius > 250 nm) and surface area concentration. The INP final products are compared with aerosol samples collected from unmanned aircraft systems (UAS) and analyzed using the ice nucleus counter FRIDGE.
Two types of particles exist in the atmosphere, primary and secondary particles. While primary particles such as soot, mineral dust, sea salt particles or pollen are introduced directly as particles into the atmosphere, secondary particles are formed in the atmosphere by condensation of gases. The formation of such new aerosol particles takes place frequently and at a broad variety of atmospheric conditions and geographic locations. A considerable fraction of the atmospheric particles is formed by such nucleation processes. The newly formed particles may grow by condensation to sizes where they are large enough to act as cloud condensation nuclei and therefore may affect cloud properties. The fundamental processes of aerosol nucleation are described and typical atmospheric observations are discussed. Two recent studies are introduced that potentially change our current understanding of atmospheric nucleation substantially.
Central and western Europe were affected by a compressional tectonic event in the Late Cretaceous, caused by the convergence of Iberia and Europe. Basement uplifts, inverted graben structures, and newly formed marginal troughs are the main expressions of crustal shortening. Although the maximum activity occurred during a short period of time between 90 and 75 Ma, the exact timing of this event is still unclear. Dating of the start and end of Late Cretaceous basin inversion gives very different results depending on the method applied. On the basis of borehole data, facies, and thickness maps, the timing of basin reorganization was reconstructed for several basins in central Europe. The obtained data point to a synchronous start of basin inversion at 95 Ma (Cenomanian), 5 Myr earlier than commonly assumed. The end of the Late Cretaceous compressional event is difficult to pinpoint in central Europe, because regional uplift and salt migration disturb the signal of shifting marginal troughs. Late Campanian to Paleogene strata deposited unconformably on inverted structures indicate slowly declining uplift rates during the latest Cretaceous. The differentiation of separate Paleogene inversion phases in central Europe does not appear possible at present.
Seeliger, Martin ; Pint, Anna ; Frenzel, Peter ; Marriner, Nick ; Spada, Giorgio ; Vacchi, Matteo ; Başaran, Sait ; Dan, Anca ; Seeger, Friederike ; Seeger, Katharina ; Schmidts, Thomas ; Brückner, Helmut
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.