11 results
Search Results
Now showing 1 - 10 of 11
- ItempH- and Temperature-Dependent Kinetics of the Oxidation Reactions of OH with Succinic and Pimelic Acid in Aqueous Solution(Basel, Switzerland : MDPI AG, 2020) Schaefer, Thomas; Wen, Liang; Estelmann, Arne; Maak, Joely; Herrmann, HartmutRate constants for the aqueous-phase reactions of the hydroxyl radical with the dicarboxylic acids, succinic acid and pimelic acid were determined using the relative rate technique over the temperature range 287 K ≤ T ≤ 318 K and at pH = 2.0, 4.6 or 4.9 and 8.0. OH radicals were generated by H2O2 laser flash photolysis while thiocyanate was used as a competitor. The pH values were adjusted to obtain the different speciation of the dicarboxylic acids. The following Arrhenius expressions were determined (in units of L mol-1 s-1): succinic acid, k(T, AH2) (2.1 x 0.1) ± 1010 exp[(-1530 x 250 K)/T], k(T, AH-) (1.8 x 0.1) ± 1010 exp[(-1070 x 370 K)/T], k(T, A2-) (2.9 x 0.2) ± 1011 exp[(-1830 x 350 K)/T] and pimelic acid, k(T, AH2) (7.3 x 0.2) ± 1010 exp[(-1040 x 140 K)/T], k(T, AH-) (1.8 x 0.1) ± 1011 exp[(-1200 x 240 K)/T], k(T, A2-) (1.4 x 0.1) ± 1012 exp[(-1830 x 110 K)/T]. A general OH radical reactivity trend for dicarboxylic acids was found as k(AH2) < k(AH-) < k(A2-). By using the pH and temperature dependent rate constants, source and sinking processes in the tropospheric aqueous phase can be described precisely. © 2020 by the authors.
- ItemDifferences and Similarities of Central Asian, African, and Arctic Dust Composition from a Single Particle Perspective(Basel, Switzerland : MDPI AG, 2020) Kandler, Konrad; Schneiders, Kilian; Heuser, Johannes; Waza, Andebo; Aryasree, Sudharaj; Althausen, Dietrich; Hofer, Julian; Abdullaev, Sabur F.; Makhmudov, Abduvosit N.Mineral dust composition affects a multitude of processes in the atmosphere and adjacent compartments. Dust dry deposition was collected near source in northwest Africa, in Central Asia, and on Svalbard and at three locations of the African outflow regime. Samples were subjected to automated scanning electron microscopy with energy-dispersive X-ray analysis to obtain size and composition of 216,000 individual particles. Results show low temporal variation in estimated optical properties for each location, but considerable differences between the African, Central Asian, and Arctic regimes. No significant difference was found between the K-feldspar relative abundances, indicating comparable related ice-nucleation abilities. The mixing state between calcium and iron compounds was different for near source and transport regimes, potentially in part due to size sorting effects. As a result, in certain situations (high acid availability, limited time) atmospheric processing of the dust is expected to lead to less increased iron solubility for near-source dusts (in particular for Central Asian ones) than for transported ones (in particular of Sahelian origin). © 2020 by the authors. Licensee MDPI, Basel, Switzerland.
- ItemPerspectives on the future of ice nucleation research: Research needs and Unanswered questions identified from two international workshops(Basel, Switzerland : MDPI AG, 2017) Coluzza, Ivan; Creamean, Jessie; Rossi, Michel J.; Wex, Heike; Alpert, Peter Aaron; Bianco, Valentino; Boose, Yvonne; Dellago, Christoph; Felgitsch, Laura; Fröhlich-Nowoisky, Janine; Herrmann, Hartmut; Jungblut, Swetlana; Kanji, Zamin A.; Menzl, Georg; Moffett, Bruce; Moritz, Clemens; Mutzel, Anke; Pöschl, Ulrich; Schauperl, Michael; Scheel, Jan; Stopelli, Emiliano; Stratmann, Frank; Grothe, Hinrich; Schmale, David G.There has been increasing interest in ice nucleation research in the last decade. To identify important gaps in our knowledge of ice nucleation processes and their impacts, two international workshops on ice nucleation were held in Vienna, Austria in 2015 and 2016. Experts from these workshops identified the following research needs: (1) uncovering the molecular identity of active sites for ice nucleation; (2) the importance of modeling for the understanding of heterogeneous ice nucleation; (3) identifying and quantifying contributions of biological ice nuclei from natural and managed environments; (4) examining the role of aging in ice nuclei; (5) conducting targeted sampling campaigns in clouds; and (6) designing lab and field experiments to increase our understanding of the role of ice-nucleating particles in the atmosphere. Interdisciplinary teams of scientists should work together to establish and maintain a common, unified language for ice nucleation research. A number of commercial applications benefit from ice nucleation research, including the production of artificial snow, the freezing and preservation of water-containing food products, and the potential modulation of weather. Additional work is needed to increase our understanding of ice nucleation processes and potential impacts on precipitation, water availability, climate change, crop health, and feedback cycles.
- ItemA Method for Retrieving Stratospheric Aerosol Extinction and Particle Size from Ground-Based Rayleigh-Mie-Raman Lidar Observations(Basel, Switzerland : MDPI AG, 2020) Zalach, Jacob; von Savigny, Christian; Langenbach, Arvid; Baumgarten, Gerd; Lübken, Franz-Josef; Bourassa, AdamWe report on the retrieval of stratospheric aerosol particle size and extinction coefficient profiles from multi-color backscatter measurements with the Rayleigh-Mie-Raman lidar operated at the Arctic Lidar Observatory for Middle Atmosphere Research (ALOMAR) in northern Norway. The retrievals are based on a two-step approach. In a first step, the median radius of an assumed monomodal log-normal particle size distribution with fixed width is retrieved based on a color index formed from the measured backscatter ratios at the wavelengths of 1064nm and 532 nm. An intrinsic ambiguity of the retrieved aerosol size information is discussed. In a second step, this particle size information is used to convert the measured lidar backscatter ratio to aerosol extinction coefficients. The retrieval is currently based on monthly-averaged lidar measurements and the results for March 2013 are discussed. A sensitivity study is presented that allows for establishing an error budget for the aerosol retrievals. Assuming a monomodal log-normal aerosol particle size distribution with a geometric width of S = 1.5, median radii on the order of below 100 nm are retrieved. The median radii are found to generally decrease with increasing altitude. The retrieved aerosol extinction profiles are compared to observations with the OSIRIS (Optical Spectrograph and InfraRed Imager System) and the OMPS-LP (Ozone Mapping Profiling Suite Limb Profiler) satellite instruments in the 60° N to 80° N latitude band. The extinction profiles that were retrieved from the lidar measurements show good agreement with the observations of the two satellite instruments when taking the different wavelengths of the instruments into account. © 2020 by the authors.
- ItemFirst results of the "Carbonaceous Aerosol in Rome and Environs (CARE)" Experiment: Beyond current standards for PM10(Basel, Switzerland : MDPI AG, 2017) Costabile, Francesca; Alas, Honey; Aufderheide, Michaela; Avino, Pasquale; Amato, Fulvio; Argentini, Stefania; Barnaba, Francesca; Berico, Massimo; Bernardoni, Vera; Biondi, Riccardo; Casasanta, Giampietro; Ciampichetti, Spartaco; Calzolai, Giulia; Canepari, Silvia; Conidi, Alessandro; Cordelli, Eugenia; Di Ianni, Antonio; Di Liberto, Luca; Facchini, Maria Cristina; Facci, Andrea; Frasca, Daniele; Gilardoni, Stefania; Grollino, Maria Giuseppa; Gualtieri, Maurizio; Lucarelli, Franco; Malaguti, Antonella; Manigrasso, Maurizio; Montagnoli, Mauro; Nava, Silvia; Perrino, Cinzia; Padoan, Elio; Petenko, Igor; Querol, Xavier; Simonetti, Giulia; Tranfo, Giovanna; Ubertini, Stefano; Valli, Gianluigi; Valentini, Sara; Vecchi, Roberta; Volpi, Francesca; Weinhold, Kay; Wiedensohler, Alfred; Zanini, Gabriele; Gobbi, Gian Paolo; Petralia, EttoreIn February 2017 the “Carbonaceous Aerosol in Rome and Environs (CARE)” experiment was carried out in downtown Rome to address the following specific questions: what is the color, size, composition, and toxicity of the carbonaceous aerosol in the Mediterranean urban background area of Rome? The motivation of this experiment is the lack of understanding of what aerosol types are responsible for the severe risks to human health posed by particulate matter (PM) pollution, and how carbonaceous aerosols influence radiative balance. Physicochemical properties of the carbonaceous aerosol were characterised, and relevant toxicological variables assessed. The aerosol characterisation includes: (i) measurements with high time resolution (min to 1–2 h) at a fixed location of black carbon (eBC), elemental carbon (EC), organic carbon (OC), particle number size distribution (0.008–10 μm), major non refractory PM1 components, elemental composition, wavelength-dependent optical properties, and atmospheric turbulence; (ii) 24-h measurements of PM10 and PM2.5 mass concentration, water soluble OC and brown carbon (BrC), and levoglucosan; (iii) mobile measurements of eBC and size distribution around the study area, with computational fluid dynamics modeling; (iv) characterisation of road dust emissions and their EC and OC content. The toxicological assessment includes: (i) preliminary evaluation of the potential impact of ultrafine particles on lung epithelia cells (cultured at the air liquid interface and directly exposed to particles); (ii) assessment of the oxidative stress induced by carbonaceous aerosols; (iii) assessment of particle size dependent number doses deposited in different regions of the human body; (iv) PAHs biomonitoring (from the participants into the mobile measurements). The first experimental results of the CARE experiment are presented in this paper. The objective here is to provide baseline levels of carbonaceous aerosols for Rome, and to address future research directions. First, we found that BC and EC mass concentration in Rome are larger than those measured in similar urban areas across Europe (the urban background mass concentration of eBC in Rome in winter being on average 2.6 ± 2.5 μg · m−3, mean eBC at the peak level hour being 5.2 (95% CI = 5.0–5.5) μg · m−3 ). Then, we discussed significant variations of carbonaceous aerosol properties occurring with time scales of minutes, and questioned on the data averaging period used in current air quality standard for PM10 (24-h). Third, we showed that the oxidative potential induced by aerosol depends on particle size and composition, the effects of toxicity being higher with lower mass concentrations and smaller particle size. Albeit this is a preliminary analysis, findings reinforce the need for an urgent update of existing air quality standards for PM10 and PM2.5 with regard to particle composition and size distribution, and data averaging period. Our results reinforce existing concerns about the toxicity of carbonaceous aerosols, support the existing evidence indicating that particle size distribution and composition may play a role in the generation of this toxicity, and remark the need to consider a shorter averaging period (<1 h) in these new standards.
- ItemDid ERA5 Improve Temperature and Precipitation Reanalysis over East Africa?(Basel, Switzerland : MDPI AG, 2020) Gleixner, Stephanie; Demissie, Teferi; Diro, Gulilat TeferaReanalysis products are often taken as an alternative solution to observational weather and climate data due to availability and accessibility problems, particularly in data-sparse regions such as Africa. Proper evaluation of their strengths and weaknesses, however, should not be overlooked. The aim of this study was to evaluate the performance of ERA5 reanalysis and to document the progress made compared to ERA-interim for the fields of near-surface temperature and precipitation over Africa. Results show that in ERA5 the climatological biases in temperature and precipitation are clearly reduced and the representation of inter-annual variability is improved over most of Africa. However, both reanalysis products performed less well in terms of capturing the observed long-term trends, despite a slightly better performance of ERA5 over ERA-interim. Further regional analysis over East Africa shows that the representation of the annual cycle of precipitation is substantially improved in ERA5 by reducing the wet bias during the rainy season. The spatial distribution of precipitation during extreme years is also better represented in ERA5. While ERA5 has improved much in comparison to its predecessor, there is still demand for improved products with even higher resolution and accuracy to satisfy impact-based studies, such as in agriculture and water resources. © 2020 by the authors.
- ItemUnmanned Aerial Systems for Investigating the Polar Atmospheric Boundary Layer—Technical Challenges and Examples of Applications(Basel, Switzerland : MDPI AG, 2020) Lampert, Astrid; Altstädter, Barbara; Bärfuss, Konrad; Bretschneider, Lutz; Sandgaard, Jesper; Michaelis, Janosch; Lobitz, Lennart; Asmussen, Magnus; Damm, Ellen; Käthner, Ralf; Krüger, Thomas; Lüpkes, Christof; Nowak, Stefan; Peuker, Alexander; Rausch, Thomas; Reiser, Fabian; Scholtz, Andreas; Zakharov, Denis Sotomayor; Gaus, Dominik; Bansmer, Stephan; Wehner, Birgit; Pätzold, FalkUnmanned aerial systems (UAS) fill a gap in high-resolution observations of meteorological parameters on small scales in the atmospheric boundary layer (ABL). Especially in the remote polar areas, there is a strong need for such detailed observations with different research foci. In this study, three systems are presented which have been adapted to the particular needs for operating in harsh polar environments: The fixed-wing aircraft M2AV with a mass of 6 kg, the quadrocopter ALICE with a mass of 19 kg, and the fixed-wing aircraft ALADINA with a mass of almost 25 kg. For all three systems, their particular modifications for polar operations are documented, in particular the insulation and heating requirements for low temperatures. Each system has completed meteorological observations under challenging conditions, including take-offand landing on the ice surface, low temperatures (down to-28 °C), icing, and, for the quadrocopter, under the impact of the rotor downwash. The influence on the measured parameters is addressed here in the form of numerical simulations and spectral data analysis. Furthermore, results from several case studies are discussed: With the M2AV, low-level flights above leads in Antarctic sea ice were performed to study the impact of areas of open water within ice surfaces on the ABL, and a comparison with simulations was performed. ALICE was used to study the small-scale structure and short-term variability of the ABL during a cruise of RV Polarstern to the 79° N glacier in Greenland. With ALADINA, aerosol measurements of different size classes were performed in Ny-Alesund, Svalbard, in highly complex terrain. In particular, very small, freshly formed particles are difficult to monitor and require the active control of temperature inside the instruments. The main aim of the article is to demonstrate the potential of UAS for ABL studies in polar environments, and to provide practical advice for future research activities with similar systems. © 2020 by the authors.
- ItemFuture Changes in Euro-Mediterranean Daytime Severe Thunderstorm Environments Based on an RCP8.5 Med-CORDEX Simulation(Basel, Switzerland : MDPI AG, 2020) Kahraman, Abdullah; Ural, Deniz; Önol, BarışConvective scale processes and, therefore, thunderstorm-related hazards cannot be simulated using regional climate models with horizontal grid spacing in the order of 10 km. However, larger-scale environmental conditions of these local high-impact phenomena can be diagnosed to assess their frequency in current and future climates. In this study, we present a daytime climatology of severe thunderstorm environments and its evolution for a wide Euro-Mediterranean domain through the 21st century, using regional climate model simulations forced by Representative Concentration Pathway (RCP) 8.5 scenario. Currently, severe convective weather is more frequently favored around Central Europe and the Mediterranean Sea. Our results suggest that with a steady progress until the end of the century, Mediterranean coasts are projected to experience a significantly higher frequency of severe thunderstorm environments, while a slight decrease over parts of continental Europe is evaluated. The increase across the Mediterranean is mostly owed to the warming sea surface, which strengthens thermodynamic conditions in the wintertime, while local factors arguably keep the shear frequency relatively higher than the entire region. On the other hand, future northward extension of the subtropical belt over Europe in the warm season reduces the number of days with severe thunderstorm environments. © 2020 by the authors.
- ItemBlack carbon aerosol in Rome (Italy): Inference of a long-term (2001-2017) record and related trends from AERONET sun-photometry data(Basel, Switzerland : MDPI AG, 2018) Di Ianni, Antonio; Costabile, Francesca; Barnaba, Francesca; Di Liberto, Luca; Weinhold, Kay; Wiedensohler, Alfred; Struckmeier, Caroline; Drewnick, Frank; Gobbi, Gian PaoloSurface concentration of black carbon (BC) is a key factor for the understanding of the impact of anthropogenic pollutants on human health. The majority of Italian cities lack long-term measurements of BC concentrations since such a metric is not regulated by EU legislation. This work attempts a long-term (2001–2017) inference of equivalent black carbon (eBC) concentrations in the city of Rome (Italy) based on sun-photometry data. To this end, aerosol light absorption coefficients at the surface are inferred from the ”columnar” aerosol aerosol light absorption coefficient records from the Rome Tor Vergata AERONET sun-photometer. The main focus of this work is to rescale aerosol light absorption columnar data (AERONET) to ground-level BC data. This is done by using values of mixing layer height (MLH) derived from ceilometer measurements and then by converting the absorption into eBC mass concentration through a mass–to–absorption conversion factor, the Mass Absorption Efficiency (MAE). The final aim is to obtain relevant data representative of the BC aerosol at the surface (i.e., in-situ)–so within the MLH– and then to infer a long-term record of “surface” equivalent black carbon mass concentration in Rome. To evaluate the accuracy of this procedure, we compared the AERONET-based results to in-situ measurements of aerosol light absorption coefficients (αabs) collected during some intensive field campaigns performed in Rome between 2010 and 2017. This analysis shows that different measurement methods, local emissions, and atmospheric conditions (MLH, residual layers) are some of the most important factors influencing differences between inferred and measured αabs. As a general result, ”inferred” and ”measured” αabs resulted to reach quite a good correlation (up to r = 0.73) after a screening procedure that excludes one of the major cause of discrepancy between AERONET inferred and in-situ measured αabs: the presence of highly absorbing aerosol layers at high altitude (e.g., dust), which frequently affects the Mediterranean site of Rome. Long-term trends of “inferred” αabs, eBC, and of the major optical variables that control aerosol’s direct radiative forcing (extinction aerosol optical depth, AODEXT, absorption aerosol optical depth, AODABS, and single scattering albedo, SSA) have been estimated. The Mann-Kendall statistical test associated with Sen’s slope was used to test the data for long-term trends. These show a negative trend for both AODEXT (−0.047/decade) and AODABS (−0.007/decade). The latter converts into a negative trend for the αabs of −5.9 Mm−1/decade and for eBC mass concentration of −0.76 μg/m3/decade. A positive trend is found for SSA (+0.014/decade), indicating that contribution of absorption to extinction is decreasing faster than that of scattering. These long-term trends are consistent with those of other air pollutant concentrations (i.e., PM2.5 and CO) in the Rome area. Despite some limitations, findings of this study fill a current lack in BC observations and may bear useful implications with regard to the improvement of our understanding of the impact of BC on air quality and climate in this Mediterranean urban region.
- ItemAerosol Particle and Black Carbon Emission Factors of Vehicular Fleet in Manila, Philippines(Basel, Switzerland : MDPI AG, 2019) Madueño, Leizel; Kecorius, Simonas; Birmili, Wolfram; Müller, Thomas; Simpas, James; Vallar, Edgar; Galvez, Maria Cecilia; Cayetano, Mylene; Wiedensohler, AlfredPoor air quality has been identified as one of the main risks to human health, especially in developing regions, where the information on physical chemical properties of air pollutants is lacking. To bridge this gap, we conducted an intensive measurement campaign in Manila, Philippines to determine the emission factors (EFs) of particle number (PN) and equivalent black carbon (BC). The focus was on public utility jeepneys (PUJ), equipped with old technology diesel engines, widely used for public transportation. The EFs were determined by aerosol physical measurements, fleet information, and modeled dilution using the Operational Street Pollution Model (OSPM). The results show that average vehicle EFs of PN and BC in Manila is up to two orders of magnitude higher than European emission standards. Furthermore, a PUJ emits up to seven times more than a light-duty vehicles (LDVs) and contribute to more than 60% of BC emission in Manila. Unfortunately, traffic restrictions for heavy-duty vehicles do not apply to PUJs. The results presented in this work provide a framework to help support targeted traffic interventions to improve urban air quality not only in Manila, but also in other countries with a similar fleet composed of old-technology vehicles. © 2019 by the authors.