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- ItemA quantification method for heat-decomposable methylglyoxal oligomers and its application on 1,3,5-trimethylbenzene SOA(Katlenburg-Lindau : EGU, 2017) Rodigast, Maria; Mutzel, Anke; Herrmann, HartmutMethylglyoxal forms oligomeric compounds in the atmospheric aqueous particle phase, which could establish a significant contribution to the formation of aqueous secondary organic aerosol (aqSOA). Thus far, no suitable method for the quantification of methylglyoxal oligomers is available despite the great effort spent for structure elucidation. In the present study a simplified method was developed to quantify heat-decomposable methylglyoxal oligomers as a sum parameter. The method is based on the thermal decomposition of oligomers into methylglyoxal monomers. Formed methylglyoxal monomers were detected using PFBHA (O-(2,3,4,5,6-pentafluorobenzyl)hydroxylamine hydrochloride) derivatisation and gas chromatography-mass spectrometry (GC/MS) analysis. The method development was focused on the heating time (varied between 15 and 48h), pH during the heating process (pH Combining double low line 1-7), and heating temperature (50, 100°C). The optimised values of these method parameters are presented. The developed method was applied to quantify heat-decomposable methylglyoxal oligomers formed during the OH-radical oxidation of 1,3,5-trimethylbenzene (TMB) in the Leipzig aerosol chamber (LEipziger AerosolKammer, LEAK). Oligomer formation was investigated as a function of seed particle acidity and relative humidity. A fraction of heat-decomposable methylglyoxal oligomers of up to 8% in the produced organic particle mass was found, highlighting the importance of those oligomers formed solely by methylglyoxal for SOA formation. Overall, the present study provides a new and suitable method for quantification of heat-decomposable methylglyoxal oligomers in the aqueous particle phase.
- ItemClassification of Arctic, midlatitude and tropical clouds in the mixed-phase temperature regime(Katlenburg-Lindau : EGU, 2017) Costa, Anja; Meyer, Jessica; Afchine, Armin; Luebke, Anna; Günther, Gebhard; Dorsey, James R.; Gallagher, Martin W.; Ehrlich, Andre; Wendisch, Manfred; Baumgardner, Darrel; Wex, Heike; Krämer, MartinaThe degree of glaciation of mixed-phase clouds constitutes one of the largest uncertainties in climate prediction. In order to better understand cloud glaciation, cloud spectrometer observations are presented in this paper, which were made in the mixed-phase temperature regime between 0 and -38°C (273 to 235K), where cloud particles can either be frozen or liquid. The extensive data set covers four airborne field campaigns providing a total of 139000 1Hz data points (38.6h within clouds) over Arctic, midlatitude and tropical regions. We develop algorithms, combining the information on number concentration, size and asphericity of the observed cloud particles to classify four cloud types: liquid clouds, clouds in which liquid droplets and ice crystals coexist, fully glaciated clouds after the Wegener-Bergeron-Findeisen process and clouds where secondary ice formation occurred. We quantify the occurrence of these cloud groups depending on the geographical region and temperature and find that liquid clouds dominate our measurements during the Arctic spring, while clouds dominated by the Wegener-Bergeron-Findeisen process are most common in midlatitude spring. The coexistence of liquid water and ice crystals is found over the whole mixed-phase temperature range in tropical convective towers in the dry season. Secondary ice is found at midlatitudes at -5 to -10°C (268 to 263K) and at higher altitudes, i.e. lower temperatures in the tropics. The distribution of the cloud types with decreasing temperature is shown to be consistent with the theory of evolution of mixed-phase clouds. With this study, we aim to contribute to a large statistical database on cloud types in the mixed-phase temperature regime.
- ItemPeakTree: A framework for structure-preserving radar Doppler spectra analysis(Göttingen : Copernicus GmbH, 2019) Radenz, M.; Bühl, J.; Seifert, P.; Griesche, H.; Engelmann, R.Clouds are frequently composed of more than one particle population even at the smallest scales. Cloud radar observations frequently contain information on multiple particle species in the observation volume when there are distinct peaks in the Doppler spectrum. Multi-peaked situations are not taken into account by established algorithms, which only use moments of the Doppler spectrum. In this study, we propose a new algorithm that recursively represents the subpeaks as nodes in a binary tree. Using this tree data structure to represent the peaks of a Doppler spectrum, it is possible to drop all a priori assumptions on the number and arrangement of subpeaks. The approach is rigid, unambiguous and can provide a basis for advanced analysis methods. The applicability is briefly demonstrated in two case studies, in which the tree structure was used to investigate particle populations in Arctic multilayered mixed-phase clouds, which were observed during the research vessel Polarstern expedition PS106 and the Atmospheric Radiation Measurement Program BAECC campaign.
- 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.
- ItemThe impact of biomass burning and aqueous-phase processing on air quality: A multi-year source apportionment study in the Po Valley, Italy(Katlenburg-Lindau : EGU, 2020) Paglione, Marco; Gilardoni, Stefania; Rinaldi, Matteo; Decesari, Stefano; Zanca, Nicola; Sandrini, Silvia; Giulianelli, Lara; Bacco, Dimitri; Ferrari, Silvia; Poluzzi, Vanes; Scotto, Fabiana; Trentini, Arianna; Poulain, Laurent; Herrmann, Hartmut; Wiedensohler, Alfred; Canonaco, Francesco; Prévôt, André S.H.; Massoli, Paola; Carbone, Claudio; Facchini, Maria Cristina; Fuzzi, SandroThe Po Valley (Italy) is a well-known air quality hotspot characterized by particulate matter (PM) levels well above the limit set by the European Air Quality Directive and by the World Health Organization, especially during the colder season. In the framework of Emilia-Romagna regional project "Supersito", the southern Po Valley submicron aerosol chemical composition was characterized by means of high-resolution aerosol mass spectroscopy (HR-AMS) with the specific aim of organic aerosol (OA) characterization and source apportionment. Eight intensive observation periods (IOPs) were carried out over 4 years (from 2011 to 2014) at two different sites (Bologna, BO, urban background, and San Pietro Capofiume, SPC, rural background), to characterize the spatial variability and seasonality of the OA sources, with a special focus on the cold season. On the multi-year basis of the study, the AMS observations show that OA accounts for averages of 45 ± 8 % (ranging from 33 % to 58 %) and 46 ± 7 % (ranging from 36 % to 50 %) of the total non-refractory submicron particle mass (PM1-NR) at the urban and rural sites, respectively. Primary organic aerosol (POA) comprises biomass burning (23±13 % of OA) and fossil fuel (12±7 %) contributions with a marked seasonality in concentration. As expected, the biomass burning contribution to POA is more significant at the rural site (urban / rural concentration ratio of 0.67), but it is also an important source of POA at the urban site during the cold season, with contributions ranging from 14 % to 38 % of the total OA mass. Secondary organic aerosol (SOA) contributes to OA mass to a much larger extent than POA at both sites throughout the year (69 ± 16 % and 83 ± 16 % at the urban and rural sites, respectively), with important implications for public health. Within the secondary fraction of OA, the measurements highlight the importance of biomass burning aging products during the cold season, even at the urban background site. This biomass burning SOA fraction represents 14 %-44 % of the total OA mass in the cold season, indicating that in this region a major contribution of combustion sources to PM mass is mediated by environmental conditions and atmospheric reactivity. © 2020 Author(s).
- ItemAerosol optical properties in the southeastern United States in summer - Part 2: Sensitivity of aerosol optical depth to relative humidity and aerosol parameters(Katlenburg-Lindau : EGU, 2016) Brock, Charles A.; Wagner, Nicholas L.; Anderson, Bruce E.; Attwood, Alexis R.; Beyersdorf, Andreas; Campuzano-Jost, Pedro; Carlton, Annmarie G.; Day, Douglas A.; Diskin, Glenn S.; Gordon, Timothy D.; Jimenez, Jose L.; Lack, Daniel A.; Liao, Jin; Markovic, Milos Z.; Middlebrook, Ann M.; Ng, Nga L.; Perring, Anne E.; Richardson, Matthews S.; Schwarz, Joshua P.; Washenfelder, Rebecca A.; Welti, Andre; Xu, Lu; Ziemba, Luke D.; Murphy, Daniel M.Aircraft observations of meteorological, trace gas, and aerosol properties were made between May and September 2013 in the southeastern United States (US). Regionally representative aggregate vertical profiles of median and interdecile ranges of the measured parameters were constructed from 37 individual aircraft profiles made in the afternoon when a well-mixed boundary layer with typical fair-weather cumulus was present (Wagner et al., 2015). We use these 0–4 km aggregate profiles and a simple model to calculate the sensitivity of aerosol optical depth (AOD) to changes in dry aerosol mass, relative humidity, mixed-layer height, the central diameter and width of the particle size distribution, hygroscopicity, and dry and wet refractive index, while holding the other parameters constant. The calculated sensitivity is a result of both the intrinsic sensitivity and the observed range of variation in these parameters. These observationally based sensitivity studies indicate that the relationship between AOD and dry aerosol mass in these conditions in the southeastern US can be highly variable and is especially sensitive to relative humidity (RH). For example, calculated AOD ranged from 0.137 to 0.305 as the RH was varied between the 10th and 90th percentile profiles with dry aerosol mass held constant. Calculated AOD was somewhat less sensitive to aerosol hygroscopicity, mean size, and geometric standard deviation, σg. However, some chemistry–climate models prescribe values of σg substantially larger than we or others observe, leading to potential high biases in model-calculated AOD of ∼ 25 %. Finally, AOD was least sensitive to observed variations in dry and wet aerosol refractive index and to changes in the height of the well-mixed surface layer. We expect these findings to be applicable to other moderately polluted and background continental air masses in which an accumulation mode between 0.1–0.5 µm diameter dominates aerosol extinction.
- ItemIs the near-spherical shape the "new black" for smoke?(Katlenburg-Lindau : EGU, 2020) Gialitaki, Anna; Tsekeri, Alexandra; Amiridis, Vassilis; Ceolato, Romain; Paulien, Lucas; Kampouri, Anna; Gkikas, Antonis; Solomos, Stavros; Marinou, Eleni; Haarig, Moritz; Baars, Holger; Ansmann, Albert; Lapyonok, Tatyana; Lopatin, Anton; Dubovik, Oleg; Groß, Silke; Wirth, Martin; Tsichla, Maria; Tsikoudi, Ioanna; Balis, DimitrisWe examine the capability of near-sphericalshaped particles to reproduce the triple-wavelength particle linear depolarization ratio (PLDR) and lidar ratio (LR) values measured over Europe for stratospheric smoke originating from Canadian wildfires. The smoke layers were detected both in the troposphere and the stratosphere, though in the latter case the particles presented PLDR values of almost 18% at 532 nm as well as a strong spectral dependence from the UV to the near-IR wavelength. Although recent simulation studies of rather complicated smoke particle morphologies have shown that heavily coated smoke aggregates can produce large PLDR, herein we propose a much simpler model of compact near-spherical smoke particles. This assumption allows for the reproduction of the observed intensive optical properties of stratospheric smoke, as well as their spectral dependence. We further examine whether an extension of the current Aerosol Robotic Network (AERONET) scattering model to include the near-spherical shapes could be of benefit to the AERONET retrieval for stratospheric smoke cases associated with enhanced PLDR. Results of our study illustrate the fact that triple-wavelength PLDR and LR lidar measurements can provide us with additional insight when it comes to particle characterization. © 2020 Author(s).
- ItemApplication of a multiple scattering model to estimate optical depth, lidar ratio and ice crystal effective radius of cirrus clouds observed with lidar.(Les Ulis : EDP Sciences, 2018) Gouveia, Diego; Baars, Holger; Seifert, Patric; Wandinger, Ulla; Barbosa, Henrique; Barja, Boris; Artaxo, Paulo; Lopes, Fabio; Landulfo, Eduardo; Ansmann, Albert; Nicolae, D.; Makoto, A.; Vassilis, A.; Balis, D.; Behrendt, A.; Comeron, A.; Gibert, F.; Landulfo, E.; McCormick, M.P.; Senff, C.; Veselovskii, I.; Wandinger, U.Lidar measurements of cirrus clouds are highly influenced by multiple scattering (MS). We therefore developed an iterative approach to correct elastic backscatter lidar signals for multiple scattering to obtain best estimates of single-scattering cloud optical depth and lidar ratio as well as of the ice crystal effective radius. The approach is based on the exploration of the effect of MS on the molecular backscatter signal returned from above cloud top.
- ItemInvestigating African trace gas sources, vertical transport, and oxidation using IAGOS-CARIBIC measurements between Germany and South Africa between 2009 and 2011(Oxford [u.a.] : Elsevier, 2017) Thorenz, U.R.; Baker, A.K.; Leedham Elvidge, E.C.; Sauvage, C.; Riede, H.; van Velthoven, P.F.J.; Hermann, M.; Weigelt, A.; Oram, D.E.; Brenninkmeijer, C.A.M.; Zahn, A.; Williams, J.Between March 2009 and March 2011 a commercial airliner equipped with a custom built measurement container (IAGOS-CARIBIC observatory) conducted 13 flights between South Africa and Germany at 10–12 km altitude, traversing the African continent north-south. In-situ measurements of trace gases (CO, CH4, H2O) and aerosol particles indicated that strong surface sources (like biomass burning) and rapid vertical transport combine to generate maximum concentrations in the latitudinal range between 10°N and 10°S coincident with the inter-tropical convergence zone (ITCZ). Pressurized air samples collected during these flights were subsequently analyzed for a suite of trace gases including C2-C8 non-methane hydrocarbons (NMHC) and halocarbons. These shorter-lived trace gases, originating from both natural and anthropogenic sources, also showed near equatorial maxima highlighting the effectiveness of convective transport in this region. Two source apportionment methods were used to investigate the specific sources of NMHC: positive matrix factorization (PMF), which is used for the first time for NMHC analysis in the upper troposphere (UT), and enhancement ratios to CO. Using the PMF method three characteristic airmass types were identified based on the different trace gas concentrations they obtained: biomass burning, fossil fuel emissions, and “background” air. The first two sources were defined with reference to previously reported surface source characterizations, while the term “background” was given to air masses in which the concentration ratios approached that of the lifetime ratios. Comparison of enhancement ratios between NMHC and CO for the subset of air samples that had experienced recent contact with the planetary boundary layer (PBL) to literature values showed that the burning of savanna and tropical forest is likely the main source of NMHC in the African upper troposphere (10–12 km). Photochemical aging patterns for the samples with PBL contact revealed that the air had different degradation histories depending on the hemisphere in which they were emitted. In the southern hemisphere (SH) air masses experienced more dilution by clean background air whereas in the northern hemisphere (NH) air masses are less diluted or mixed with background air still containing longer lived NMHC. Using NMHC photochemical clocks ozone production was seen in the BB outflow above Africa in the NH.
- ItemMeasurements of particle backscatter, extinction, and lidar ratio at 1064 nm with the rotational raman method in Polly-XT(Les Ulis : EDP Sciences, 2018) Engelmann, Ronny; Haarig, Moritz; Baars, Holger; Ansmann, Albert; Kottas, Michael; Marinou, Eleni; Nicolae, D.; Makoto, A.; Vassilis, A.; Balis, D.; Behrendt, A.; Comeron, A.; Gibert, F.; Landulfo, E.; McCormick, M.P.; Senff, C.; Veselovskii, I.; Wandinger, U.We replaced a 1064-nm interference filter of a Polly-XT lidar system by a 1058-nm filter to observe pure rotational Raman backscattering from atmospheric Nitrogen and Oxygen. Polly-XT is compact Raman lidar with a Nd:YAG laser (20 Hz, 200 mJ at 1064 nm) and a 30-cm telescope mirror which applies photomultipliers in photoncounting mode. We present the first measured signals at 1058 nm and the derived extinction profile from measurements aboard RV Polarstern and in Leipzig. In combination with another Polly-XT system we could also derive particle backscatter and lidar ratio profiles at 1064 nm.