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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.
- 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.
- ItemIce nucleating particles over the Eastern Mediterranean measured by unmanned aircraft systems(Katlenburg-Lindau : EGU, 2017) Schrod, Jann; Weber, Daniel; Drücke, Jaqueline; Keleshis, Christos; Pikridas, Michael; Ebert, Martin; Cvetković, Bojan; Nickovic, Slobodan; Marinou, Eleni; Baars, Holger; Ansmann, Albert; Vrekoussis, Mihalis; Mihalopoulos, Nikos; Sciare, Jean; Curtius, Joachim; Bingemer, Heinz G.During an intensive field campaign on aerosol, clouds, and ice nucleation in the Eastern Mediterranean in April 2016, we measured the abundance of ice nucleating particles (INPs) in the lower troposphere from unmanned aircraft systems (UASs). Aerosol samples were collected by miniaturized electrostatic precipitators onboard the UASs at altitudes up to 2.5 km. The number of INPs in these samples, which are active in the deposition and condensation modes at temperatures from -20 to -30 °C, were analyzed immediately after collection on site using the ice nucleus counter FRIDGE (FRankfurt Ice nucleation Deposition freezinG Experiment). During the 1-month campaign, we encountered a series of Saharan dust plumes that traveled at several kilometers' altitude. Here we present INP data from 42 individual flights, together with aerosol number concentrations, observations of lidar backscattering, dust concentrations derived by the dust transport model DREAM (Dust Regional Atmospheric Model), and results from scanning electron microscopy. The effect of the dust plumes is reflected by the coincidence of INPs with the particulate matter (PM), the lidar signal, and the predicted dust mass of the model. This suggests that mineral dust or a constituent related to dust was a major contributor to the ice nucleating properties of the aerosol. Peak concentrations of above 100 INPs std L-1 were measured at -30 °C. The INP concentration in elevated plumes was on average a factor of 10 higher than at ground level. Since desert dust is transported for long distances over wide areas of the globe predominantly at several kilometers' altitude, we conclude that INP measurements at ground level may be of limited significance for the situation at the level of cloud formation.
- ItemStatus and future of numerical atmospheric aerosol prediction with a focus on data requirements(Katlenburg-Lindau : EGU, 2018) Benedetti, Angela; Reid, Jeffrey S.; Knippertz, Peter; Marsham, John H.; Di Giuseppe, Francesca; Rémy, Samuel; Basart, Sara; Boucher, Olivier; Brooks, Ian M.; Menut, Laurent; Mona, Lucia; Laj, Paolo; Pappalardo, Gelsomina; Wiedensohler, Alfred; Baklanov, Alexander; Brooks, Malcolm; Colarco, Peter R.; Cuevas, Emilio; da Silva, Arlindo; Escribano, Jeronimo; Flemming, Johannes; Huneeus, Nicolas; Jorba, Oriol; Kazadzis, Stelios; Kinne, Stefan; Popp, Thomas; Quinn, Patricia K.; Sekiyama, Thomas T.; Tanaka, Taichu; Terradellas, EnricNumerical prediction of aerosol particle properties has become an important activity at many research and operational weather centers. This development is due to growing interest from a diverse set of stakeholders, such as air quality regulatory bodies, aviation and military authorities, solar energy plant managers, climate services providers, and health professionals. Owing to the complexity of atmospheric aerosol processes and their sensitivity to the underlying meteorological conditions, the prediction of aerosol particle concentrations and properties in the numerical weather prediction (NWP) framework faces a number of challenges. The modeling of numerous aerosol-related parameters increases computational expense. Errors in aerosol prediction concern all processes involved in the aerosol life cycle including (a) errors on the source terms (for both anthropogenic and natural emissions), (b) errors directly dependent on the meteorology (e.g., mixing, transport, scavenging by precipitation), and (c) errors related to aerosol chemistry (e.g., nucleation, gas-aerosol partitioning, chemical transformation and growth, hygroscopicity). Finally, there are fundamental uncertainties and significant processing overhead in the diverse observations used for verification and assimilation within these systems. Indeed, a significant component of aerosol forecast development consists in streamlining aerosol-related observations and reducing the most important errors through model development and data assimilation. Aerosol particle observations from satellite- and ground-based platforms have been crucial to guide model development of the recent years and have been made more readily available for model evaluation and assimilation. However, for the sustainability of the aerosol particle prediction activities around the globe, it is crucial that quality aerosol observations continue to be made available from different platforms (space, near surface, and aircraft) and freely shared. This paper reviews current requirements for aerosol observations in the context of the operational activities carried out at various global and regional centers. While some of the requirements are equally applicable to aerosol-climate, the focus here is on global operational prediction of aerosol properties such as mass concentrations and optical parameters. It is also recognized that the term "requirements" is loosely used here given the diversity in global aerosol observing systems and that utilized data are typically not from operational sources. Most operational models are based on bulk schemes that do not predict the size distribution of the aerosol particles. Others are based on a mix of "bin" and bulk schemes with limited capability of simulating the size information. However the next generation of aerosol operational models will output both mass and number density concentration to provide a more complete description of the aerosol population. A brief overview of the state of the art is provided with an introduction on the importance of aerosol prediction activities. The criteria on which the requirements for aerosol observations are based are also outlined. Assimilation and evaluation aspects are discussed from the perspective of the user requirements.
- ItemA parameterization of the heterogeneous hydrolysis of N2O5 for mass-based aerosol models: Improvement of particulate nitrate prediction(Katlenburg-Lindau : EGU, 2018) Chen, Ying; Wolke, Ralf; Ran, Liang; Birmili, Wolfram; Spindler, Gerald; Schröder, Wolfram; Su, Hang; Cheng, Yafang; Tegen, Ina; Wiedensohler, AlfredThe heterogeneous hydrolysis of N2O5 on the surface of deliquescent aerosol leads to HNO3 formation and acts as a major sink of NOx in the atmosphere during night-time. The reaction constant of this heterogeneous hydrolysis is determined by temperature (T), relative humidity (RH), aerosol particle composition, and the surface area concentration (S). However, these parameters were not comprehensively considered in the parameterization of the heterogeneous hydrolysis of N2O5 in previous mass-based 3-D aerosol modelling studies. In this investigation, we propose a sophisticated parameterization (NewN2O5) of N2O5 heterogeneous hydrolysis with respect to T, RH, aerosol particle compositions, and S based on laboratory experiments. We evaluated closure between NewN2O5 and a state-of-the-art parameterization based on a sectional aerosol treatment. The comparison showed a good linear relationship (R Combining double low line 0.91) between these two parameterizations. NewN2O5 was incorporated into a 3-D fully online coupled model, COSMO-Muscat, with the mass-based aerosol treatment. As a case study, we used the data from the HOPE Melpitz campaign (10-25 September 2013) to validate model performance. Here, we investigated the improvement of nitrate prediction over western and central Europe. The modelled particulate nitrate mass concentrations ([NO3-]) were validated by filter measurements over Germany (Neuglobsow, Schmücke, Zingst, and Melpitz). The modelled [NO3-] was significantly overestimated for this period by a factor of 5-19, with the corrected NH3 emissions (reduced by 50 %) and the original parameterization of N2O5 heterogeneous hydrolysis. The NewN2O5 significantly reduces the overestimation of [NO3-] by ∼ 35 %. Particularly, the overestimation factor was reduced to approximately 1.4 in our case study (12, 17-18 and 25 September 2013) when [NO3-] was dominated by local chemical formations. In our case, the suppression of organic coating was negligible over western and central Europe, with an influence on [NO3-] of less than 2 % on average and 20 % at the most significant moment. To obtain a significant impact of the organic coating effect, N2O5, SOA, and NH3 need to be present when RH is high and T is low. However, those conditions were rarely fulfilled simultaneously over western and central Europe. Hence, the organic coating effect on the reaction probability of N2O5 may not be as significant as expected over western and central Europe.
- ItemSecondary organic aerosol (SOA) yields from NO3 radical + isoprene based on nighttime aircraft power plant plume transects(Katlenburg-Lindau : EGU, 2018) Fry, Juliane L.; Brown, Steven S.; Middlebrook, Ann M.; Edwards, Peter M.; Campuzano-Jost, Pedro; Day, Douglas A.; Jimenez, José L.; Allen, Hannah M.; Ryerson, Thomas B.; Pollack, Ilana; Graus, Martin; Warneke, Carsten; de Gouw, Joost A.; Brock, Charles A.; Gilman, Jessica; Lerner, Brian M.; Dubé, William P.; Liao, Jin; Welti, AndréNighttime reaction of nitrate radicals (NO3) with biogenic volatile organic compounds (BVOC) has been proposed as a potentially important but also highly uncertain source of secondary organic aerosol (SOA). The southeastern United States has both high BVOC and nitrogen oxide (NOx) emissions, resulting in a large model-predicted NO3-BVOC source of SOA. Coal-fired power plants in this region constitute substantial NOx emissions point sources into a nighttime atmosphere characterized by high regionally widespread concentrations of isoprene. In this paper, we exploit nighttime aircraft observations of these power plant plumes, in which NO3 radicals rapidly remove isoprene, to obtain field-based estimates of the secondary organic aerosol yield from NO3 + isoprene. Observed in-plume increases in nitrate aerosol are consistent with organic nitrate aerosol production from NO3 + isoprene, and these are used to determine molar SOA yields, for which the average over nine plumes is 9 % (±5 %). Corresponding mass yields depend on the assumed molecular formula for isoprene-NO3-SOA, but the average over nine plumes is 27 % (±14 %), on average larger than those previously measured in chamber studies (12 %-14 % mass yield as ΔOA / ΔVOC after oxidation of both double bonds). Yields are larger for longer plume ages. This suggests that ambient aging processes lead more effectively to condensable material than typical chamber conditions allow. We discuss potential mechanistic explanations for this difference, including longer ambient peroxy radical lifetimes and heterogeneous reactions of NO3-isoprene gas phase products. More in-depth studies are needed to better understand the aerosol yield and oxidation mechanism of NO3 radical + isoprene, a coupled anthropogenic-biogenic source of SOA that may be regionally significant.
- ItemSatellite retrievals of dust aerosol over the Red Sea and the Persian Gulf (2005-2015)(Katlenburg-Lindau : EGU, 2017) Banks, Jamie R.; Brindley, Helen E.; Stenchikov, Georgiy; Schepanski, KerstinThe inter-annual variability of the dust aerosol presence over the Red Sea and the Persian Gulf is analysed over the period 2005-2015. Particular attention is paid to the variation in loading across the Red Sea, which has previously been shown to have a strong, seasonally dependent latitudinal gradient. Over the 11 years considered, the July mean 630 nm aerosol optical depth (AOD) derived from the Spinning Enhanced Visible and InfraRed Imager (SEVIRI) varies between 0.48 and 1.45 in the southern half of the Red Sea. In the north, the equivalent variation is between 0.22 and 0.66. The temporal and spatial pattern of variability captured by SEVIRI is also seen in AOD retrievals from the MODerate Imaging Spectroradiometer (MODIS), but there is a systematic offset between the two records. Comparisons of both sets of retrievals with ship-and land-based AERONET measurements show a high degree of correlation with biases of <0.08. However, these comparisons typically only sample relatively low aerosol loadings. When both records are stratified by AOD retrievals from the Multi-angle Imaging SpectroRadiometer (MISR), opposing behaviour is revealed at high MISR AODs (>1), with offsets of C0.19 for MODIS and 0.06 for SEVIRI. Similar behaviour is also seen over the Persian Gulf. Analysis of the scattering angles at which retrievals from the SEVIRI and MODIS measurements are typically performed in these regions suggests that assumptions concerning particle sphericity may be responsible for the differences seen.
- ItemRemote sensing and modelling analysis of the extreme dust storm hitting the Middle East and eastern Mediterranean in September 2015(Katlenburg-Lindau : EGU, 2017) Solomos, Stavros; Ansmann, Albert; Mamouri, Rodanthi-Elisavet; Binietoglou, Ioannis; Patlakas, Platon; Marinou, Eleni; Amiridis, VassilisThe extreme dust storm that affected the Middle East and the eastern Mediterranean in September 2015 resulted in record-breaking dust loads over Cyprus with aerosol optical depth exceeding 5.0 at 550ĝ€nm. We analyse this event using profiles from the European Aerosol Research Lidar Network (EARLINET) and the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO), geostationary observations from the Meteosat Second Generation (MSG) Spinning Enhanced Visible and Infrared Imager (SEVIRI), and high-resolution simulations from the Regional Atmospheric Modeling System (RAMS). The analysis of modelling and remote sensing data reveals the main mechanisms that resulted in the generation and persistence of the dust cloud over the Middle East and Cyprus. A combination of meteorological and surface processes is found, including (a) the development of a thermal low in the area of Syria that results in unstable atmospheric conditions and dust mobilization in this area, (b) the convective activity over northern Iraq that triggers the formation of westward-moving haboobs that merge with the previously elevated dust layer, and (c) the changes in land use due to war in the areas of northern Iraq and Syria that enhance dust erodibility.
- ItemDetection and attribution of aerosol-cloud interactions in large-domain large-eddy simulations with the ICOsahedral Non-hydrostatic model(Katlenburg-Lindau : EGU, 2020) Costa-Surós, Montserrat; Sourdeval, Odran; Acquistapace, Claudia; Baars, Holger; Carbajal Henken, Cintia; Genz, Christa; Hesemann, Jonas; Jimenez, Cristofer; König, Marcel; Kretzschmar, Jan; Madenach, Nils; Meyer, Catrin I.; Schrödner, Roland; Seifert, Patric; Senf, Fabian; Brueck, Matthias; Cioni, Guido; Engels, Jan Frederik; Fieg, Kerstin; Gorges, Ksenia; Heinze, Rieke; Kumar Siligam, Pavan; Burkhardt, Ulrike; Crewell, Susanne; Hoose, Corinna; Seifert, Axel; Tegen, Ina; Quaas, JohannesClouds and aerosols contribute the largest uncertainty to current estimates and interpretations of the Earth's changing energy budget. Here we use a new-generation large-domain large-eddy model, ICON-LEM (ICOsahedral Non-hydrostatic Large Eddy Model), to simulate the response of clouds to realistic anthropogenic perturbations in aerosols serving as cloud condensation nuclei (CCN). The novelty compared to previous studies is that (i) the LEM is run in weather prediction mode and with fully interactive land surface over a large domain and (ii) a large range of data from various sources are used for the detection and attribution. The aerosol perturbation was chosen as peak-aerosol conditions over Europe in 1985, with more than fivefold more sulfate than in 2013. Observational data from various satellite and ground-based remote sensing instruments are used, aiming at the detection and attribution of this response. The simulation was run for a selected day (2 May 2013) in which a large variety of cloud regimes was present over the selected domain of central Europe. It is first demonstrated that the aerosol fields used in the model are consistent with corresponding satellite aerosol optical depth retrievals for both 1985 (perturbed) and 2013 (reference) conditions. In comparison to retrievals from groundbased lidar for 2013, CCN profiles for the reference conditions were consistent with the observations, while the ones for the 1985 conditions were not. Similarly, the detection and attribution process was successful for droplet number concentrations: the ones simulated for the 2013 conditions were consistent with satellite as well as new ground-based lidar retrievals, while the ones for the 1985 conditions were outside the observational range. For other cloud quantities, including cloud fraction, liquid water path, cloud base altitude and cloud lifetime, the aerosol response was small compared to their natural vari ability. Also, large uncertainties in satellite and ground-based observations make the detection and attribution difficult for these quantities. An exception to this is the fact that at a large liquid water path value (LWP > 200 g m-2), the control simulation matches the observations, while the perturbed one shows an LWP which is too large. The model simulations allowed for quantifying the radiative forcing due to aerosol-cloud interactions, as well as the adjustments to this forcing. The latter were small compared to the variability and showed overall a small positive radiative effect. The overall effective radiative forcing (ERF) due to aerosol-cloud interactions (ERFaci) in the simulation was dominated thus by the Twomey effect and yielded for this day, region and aerosol perturbation-2:6 W m-2. Using general circulation models to scale this to a global-mean present-day vs. pre-industrial ERFaci yields a global ERFaci of-0:8 W m-2 © 2020 Author(s).