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- ItemCharacterization of organic aerosol across the global remote troposphere: A comparison of ATom measurements and global chemistry models(Katlenburg-Lindau : EGU, 2020) Hodzic, Alma; Campuzano-Jost, Pedro; Bian, Huisheng; Chin, Mian; Colarco, Peter R.; Day, Douglas A.; Froyd, Karl D.; Heinold, Bernd; Katich, Joseph M.; Jo, Duseong S.; Kodros, John K.; Nault, Benjamin A.; Pierce, Jeffrey R.; Ray, Eric; Schacht, Jacob; Schill, Gregory P.; Schroder, Jason C.; Schwarz, Joshua P.; Sueper, Donna T.; Tegen, Ina; Tilmes, Simone; Tsigaridis, Kostas; Yu, Pengfei; Jimenez, Jose L.The spatial distribution and properties of submicron organic aerosol (OA) are among the key sources of uncertainty in our understanding of aerosol effects on climate. Uncertainties are particularly large over remote regions of the free troposphere and Southern Ocean, where very few data have been available and where OA predictions from AeroCom Phase II global models span 2 to 3 orders of magnitude, greatly exceeding the model spread over source regions. The (nearly) pole-to-pole vertical distribution of nonrefractory aerosols was measured with an aerosol mass spectrometer onboard the NASA DC-8 aircraft as part of the Atmospheric Tomography (ATom) mission during the Northern Hemisphere summer (August 2016) and winter (February 2017). This study presents the first extensive characterization of OA mass concentrations and their level of oxidation in the remote atmosphere. OA and sulfate are the major contributors by mass to submicron aerosols in the remote troposphere, together with sea salt in the marine boundary layer. Sulfate was dominant in the lower stratosphere. OA concentrations have a strong seasonal and zonal variability, with the highest levels measured in the lower troposphere in the summer and over the regions influenced by biomass burning from Africa (up to 10 μgsm-3). Lower concentrations (~ 0:1 0.3 μgsm-3) are observed in the northern middle and high latitudes and very low concentrations (< 0:1 μgsm-3) in the southern middle and high latitudes. The ATom dataset is used to evaluate predictions of eight current global chemistry models that implement a variety of commonly used representations of OA sources and chemistry, as well as of the AeroCom-II ensemble. The current model ensemble captures the average vertical and spatial distribution of measured OA concentrations, and the spread of the individual models remains within a factor of 5. These results are significantly improved over the AeroCom-II model ensemble, which shows large overestimations over these regions. However, some of the improved agreement with observations occurs for the wrong reasons, as models have the tendency to greatly overestimate the primary OA fraction and underestimate the sec-ondary fraction. Measured OA in the remote free troposphere is highly oxygenated, with organic aerosol to organic carbon (OA= OC) ratios of ~ 2.2 2.8, and is 30 % 60% more oxygenated than in current models, which can lead to significant errors in OA concentrations. The model measurement comparisons presented here support the concept of a more dynamic OA system as proposed by Hodzic et al. (2016), with enhanced removal of primary OA and a stronger production of secondary OA in global models needed to provide better agreement with observations. © 2020 IEEE Computer Society. All rights reserved.
- ItemOrganic aerosol components derived from 25 AMS data sets across Europe using a consistent ME-2 based source apportionment approach(München : European Geopyhsical Union, 2014) Crippa, M.; Canonaco, F.; Lanz, V.A.; Äijälä, M.; Allan, J.D.; Carbone, S.; Capes, G.; Ceburnis, D.; Dall'Osto, M.; Day, D.A.; DeCarlo, P.F.; Ehn, M.; Eriksson, A.; Freney, E.; Hildebrandt Ruiz, L.; Hillamo, R.; Jimenez, J.L.; Junninen, H.; Kiendler-Scharr, A.; Kortelainen, A.-M.; Kulmala, M.; Laaksonen, A.; Mensah, A.A.; Mohr, C.; Nemitz, E.; O'Dowd, C.; Ovadnevaite, J.; Pandis, S.N.; Petäjä, T.; Poulain, L.; Saarikoski, S.; Sellegri, K.; Swietlicki, E.; Tiitta, P.; Worsnop, D.R.; Baltensperger, U.; Prévôt, A.S.H.Organic aerosols (OA) represent one of the major constituents of submicron particulate matter (PM1) and comprise a huge variety of compounds emitted by different sources. Three intensive measurement field campaigns to investigate the aerosol chemical composition all over Europe were carried out within the framework of the European Integrated Project on Aerosol Cloud Climate and Air Quality Interactions (EUCAARI) and the intensive campaigns of European Monitoring and Evaluation Programme (EMEP) during 2008 (May–June and September–October) and 2009 (February–March). In this paper we focus on the identification of the main organic aerosol sources and we define a standardized methodology to perform source apportionment using positive matrix factorization (PMF) with the multilinear engine (ME-2) on Aerodyne aerosol mass spectrometer (AMS) data. Our source apportionment procedure is tested and applied on 25 data sets accounting for two urban, several rural and remote and two high altitude sites; therefore it is likely suitable for the treatment of AMS-related ambient data sets. For most of the sites, four organic components are retrieved, improving significantly previous source apportionment results where only a separation in primary and secondary OA sources was possible. Generally, our solutions include two primary OA sources, i.e. hydrocarbon-like OA (HOA) and biomass burning OA (BBOA) and two secondary OA components, i.e. semi-volatile oxygenated OA (SV-OOA) and low-volatility oxygenated OA (LV-OOA). For specific sites cooking-related (COA) and marine-related sources (MSA) are also separated. Finally, our work provides a large overview of organic aerosol sources in Europe and an interesting set of highly time resolved data for modeling purposes.
- ItemEvolution of particle composition in CLOUD nucleation experiments(München : European Geopyhsical Union, 2013) Keskinen, H.; Virtanen, A.; Joutsensaari, J.; Tsagkogeorgas, G.; Duplissy, J.; Schobesberger, S.; Gysel, M.; Riccobono, F.; Slowik, J.G.; Bianchi, F.; Yli-Juuti, T.; Lehtipalo, K.; Rondo, L.; Breitenlechner, M.; Kupc, A.; Almeida, J.; Amorim, A.; Dunne, E.M.; Downard, A.J.; Ehrhart, S.; Franchin, A.; Kajos, M.K.; Kirkby, J.; Kürten, A.; Nieminen, T.; Makhmutov, V.; Mathot, S.; Miettinen, P.; Onnela, A.; Petäjä, T.; Praplan, A.; Santos, F.D.; Schallhart, S.; Sipilä, M.; Stozhkov, Y.; Tomé, A.; Vaattovaara, P.; Wimmer, D.; Prevot, A.; Dommen, J.; Donahue, N.M.; Flagan, R.C.; Weingartner, E.; Viisanen, Y.; Riipinen, I.; Hansel, A.; Curtius, J.; Kulmala, M.; Worsnop, D.R.; Baltensperger, U.; Wex, H.; Stratmann, F.; Laaksonen, A.Sulphuric acid, ammonia, amines, and oxidised organics play a crucial role in nanoparticle formation in the atmosphere. In this study, we investigate the composition of nucleated nanoparticles formed from these compounds in the CLOUD (Cosmics Leaving Outdoor Droplets) chamber experiments at CERN (Centre européen pour la recherche nucléaire). The investigation was carried out via analysis of the particle hygroscopicity, ethanol affinity, oxidation state, and ion composition. Hygroscopicity was studied by a hygroscopic tandem differential mobility analyser and a cloud condensation nuclei counter, ethanol affinity by an organic differential mobility analyser and particle oxidation level by a high-resolution time-of-flight aerosol mass spectrometer. The ion composition was studied by an atmospheric pressure interface time-of-flight mass spectrometer. The volume fraction of the organics in the particles during their growth from sizes of a few nanometers to tens of nanometers was derived from measured hygroscopicity assuming the Zdanovskii–Stokes–Robinson relationship, and compared to values gained from the spectrometers. The ZSR-relationship was also applied to obtain the measured ethanol affinities during the particle growth, which were used to derive the volume fractions of sulphuric acid and the other inorganics (e.g. ammonium salts). In the presence of sulphuric acid and ammonia, particles with a mobility diameter of 150 nm were chemically neutralised to ammonium sulphate. In the presence of oxidation products of pinanediol, the organic volume fraction of freshly nucleated particles increased from 0.4 to ~0.9, with an increase in diameter from 2 to 63 nm. Conversely, the sulphuric acid volume fraction decreased from 0.6 to 0.1 when the particle diameter increased from 2 to 50 nm. The results provide information on the composition of nucleated aerosol particles during their growth in the presence of various combinations of sulphuric acid, ammonia, dimethylamine and organic oxidation products.
- ItemDiurnal variations of aerosol optical properties in the North China Plain and their influences on the estimates of direct aerosol radiative effect(München : European Geopyhsical Union, 2015) Kuang, Y.; Zhao, C.S.; Tao, J.C.; Ma, N.In this paper, the diurnal variations of aerosol optical properties and their influences on the estimation of daily average direct aerosol radiative effect (DARE) in the North China Plain (NCP) are investigated based on in situ measurements from Haze in China campaign. For ambient aerosol, the diurnal patterns of single scattering albedo (SSA) and asymmetry factor (g) in the NCP are both highest at dawn and lowest in the late afternoon, and quite different from those of dry-state aerosol. The relative humidity (RH) is the dominant factor which determines the diurnal pattern of SSA and g for ambient aerosol. Basing on the calculated SSA and g, several cases are designed to investigate the impacts of the diurnal changes of aerosol optical properties on DARE. The results demonstrate that the diurnal changes of SSA and g in the NCP have significant influences on the estimation of DARE at the top of the atmosphere (TOA). If the full temporal coverage of aerosol optical depth (AOD), SSA and g are available, an accurate estimation of daily average DARE can be achieved by using the daily averages of AOD, SSA and g. However, due to the lack of full temporal coverage data sets of SSA and g, their daily averages are usually not available. Basing on the results of designed cases, if the RH plays a dominant role in the diurnal variations of SSA and g, we suggest that using both SSA and g averaged over early morning and late afternoon as inputs for radiative transfer model to improve the accurate estimation of DARE. If the temporal samplings of SSA or g are too few to adopt this method, either averaged over early morning or late afternoon of both SSA and g can be used to improve the estimation of DARE at the TOA.
- ItemAnalysis of nucleation events in the European boundary layer using the regional aerosol-climate model REMO-HAM with a solar radiation-driven OH-proxy(München : European Geopyhsical Union, 2014) Pietikäinen, J.-P.; Mikkonen, S.; Hamed, A.; Hienola, A.I.; Birmili, W.; Kulmala, M.; Laaksonen, A.This work describes improvements in the regional aerosol–climate model REMO-HAM in order to simulate more realistically the process of atmospheric new particle formation (NPF). A new scheme was implemented to simulate OH radical concentrations using a proxy approach based on observations and also accounting for the effects of clouds upon OH concentrations. Second, the nucleation rate calculation was modified to directly simulate the formation rates of 3 nm particles, which removes some unnecessary steps in the formation rate calculations used earlier in the model. Using the updated model version, NPF over Europe was simulated for the periods 2003–2004 and 2008–2009. The statistics of the simulated particle formation events were subsequently compared to observations from 13 ground-based measurement sites. The new model shows improved agreement with the observed NPF rates compared to former versions and can simulate the event statistics realistically for most parts of Europe.
- ItemAerosol particle measurements at three stationary sites in the megacity of Paris during summer 2009: Meteorology and air mass origin dominate aerosol particle composition and size distribution(München : European Geopyhsical Union, 2013) Freutel, F.; Schneider, J.; Drewnick, F.; Weiden-Reinmüller, S.-L.; Crippa, M.; Prévôt, A.S.H.; Baltensperger, U.; Poulain, L.; Wiedensohler, R.A.; Sciare, J.; Sarda-Estève, R.; Burkhart, J.F.; Eckhardt, S.; Stohl, A.; Gros, V.; Colomb, A.; Michoud, V.; Doussin, J.F.; Borbon, A.; Haeffelin, M.; Morille, Y.; Beekmann, M.; Borrmann, S.During July 2009, a one-month measurement campaign was performed in the megacity of Paris. Amongst other measurement platforms, three stationary sites distributed over an area of 40 km in diameter in the greater Paris region enabled a detailed characterization of the aerosol particle and gas phase. Simulation results from the FLEXPART dispersion model were used to distinguish between different types of air masses sampled. It was found that the origin of air masses had a large influence on measured mass concentrations of the secondary species particulate sulphate, nitrate, ammonium, and oxygenated organic aerosol measured with the Aerodyne aerosol mass spectrometer in the submicron particle size range: particularly high concentrations of these species (about 4 μg m−3, 2 μg m−3, 2 μg m−3, and 7 μg m−3, respectively) were measured when aged material was advected from continental Europe, while for air masses originating from the Atlantic, much lower mass concentrations of these species were observed (about 1 μg m−3, 0.2 μg m−3, 0.4 μg m−3, and 1–3 μg m−3, respectively). For the primary emission tracers hydrocarbon-like organic aerosol, black carbon, and NOx it was found that apart from diurnal source strength variations and proximity to emission sources, local meteorology had the largest influence on measured concentrations, with higher wind speeds leading to larger dilution and therefore smaller measured concentrations. Also the shape of particle size distributions was affected by wind speed and air mass origin. Quasi-Lagrangian measurements performed under connected flow conditions between the three stationary sites were used to estimate the influence of the Paris emission plume onto its surroundings, which was found to be rather small. Rough estimates for the impact of the Paris emission plume on the suburban areas can be inferred from these measurements: Volume mixing ratios of 1–14 ppb of NOx, and upper limits for mass concentrations of about 1.5 μg m−3 of black carbon and of about 3 μg m−3 of hydrocarbon-like organic aerosol can be deduced which originate from both, local emissions and the overall Paris emission plume. The secondary aerosol particle phase species were found to be not significantly influenced by the Paris megacity, indicating their regional origin. The submicron aerosol mass concentrations of particulate sulphate, nitrate, and ammonium measured during time periods when air masses were advected from eastern central Europe were found to be similar to what has been found from other measurement campaigns in Paris and south-central France for this type of air mass origin, indicating that the results presented here are also more generally valid.
- ItemHygroscopic properties of the Paris urban aerosol in relation to its chemical composition(München : European Geopyhsical Union, 2014) Kamilli, K.A.; Poulain, L.; Held, A.; Nowak, A.; Birmili, W.; Wiedensohler, A.Aerosol hygroscopic growth factors and chemical properties were measured as part of the MEGAPOLI "Megacities Plume Case Study" at the urban site Laboratoire d'Hygiène de la Ville de Paris (LHVP) in the city center of Paris from June to August 2009, and from January to February 2010. Descriptive hygroscopic growth factors (DGF) were derived in the diameter range from 25 to 350 nm at relative humidities of 30, 55, 75, and 90% by applying the summation method on humidified and dry aerosol size distributions measured simultaneously with a humidified differential mobility particle sizer (HDMPS) and a twin differential mobility particle sizer (TDMPS). For 90% relative humidity, the DGF varied from 1.06 to 1.46 in summer, and from 1.06 to 1.66 in winter. Temporal variations in the observed mean DGF could be well explained with a simple growth model based on the aerosol chemical composition measured by aerosol mass spectrometry (AMS) and black carbon photometry (MAAP). In particular, good agreement was observed when sulfate was the predominant inorganic factor. A clear overestimation of the predicted growth factor was found when the nitrate mass concentration exceeded values of 10 μg m−3, e.g., during winter.
- ItemRegional effects of atmospheric aerosols on temperature: An evaluation of an ensemble of online coupled models(Katlenburg-Lindau : EGU, 2017) Baró, Rocío; Palacios-Peña, Laura; Baklanov, Alexander; Balzarini, Alessandra; Brunner, Dominik; Forkel, Renate; Hirtl, Marcus; Honzak, Luka; Pérez, Juan Luis; Pirovano, Guido; San José, Roberto; Schröder, Wolfram; Werhahn, Johannes; Wolke, Ralf; Žabkar, Rahela; Jiménez-Guerrero, PedroThe climate effect of atmospheric aerosols is associated with their influence on the radiative budget of the Earth due to the direct aerosol-radiation interactions (ARIs) and indirect effects, resulting from aerosol-cloud-radiation interactions (ACIs). Online coupled meteorology-chemistry models permit the description of these effects on the basis of simulated atmospheric aerosol concentrations, although there is still some uncertainty associated with the use of these models. Thus, the objective of this work is to assess whether the inclusion of atmospheric aerosol radiative feedbacks of an ensemble of online coupled models improves the simulation results for maximum, mean and minimum temperature at 2m over Europe. The evaluated models outputs originate from EuMetChem COST Action ES1004 simulations for Europe, differing in the inclusion (or omission) of ARI and ACI in the various models. The cases studies cover two important atmospheric aerosol episodes over Europe in the year 2010: (i) a heat wave event and a forest fire episode (July-August 2010) and (ii) a more humid episode including a Saharan desert dust outbreak in October 2010. The simulation results are evaluated against observational data from the E-OBS gridded database. The results indicate that, although there is only a slight improvement in the bias of the simulation results when including the radiative feedbacks, the spatiotemporal variability and correlation coefficients are improved for the cases under study when atmospheric aerosol radiative effects are included.
- ItemAerosol hygroscopicity derived from size-segregated chemical composition and its parameterization in the North China Plain(München : European Geopyhsical Union, 2014) Liu, H.J.; Zhao, C.S.; Nekat, B.; Ma, N.; Wiedensohler, A.; van Pinxteren, D.; Spindler, G.; Müller, K.; Herrmann, H.Hygroscopic growth of aerosol particles is of significant importance in quantifying the aerosol radiative effect in the atmosphere. In this study, hygroscopic properties of ambient particles are investigated based on particle chemical composition at a suburban site in the North China Plain during the HaChi campaign (Haze in China) in summer 2009. The size-segregated aerosol particulate mass concentration as well as the particle components such as inorganic ions, organic carbon and water-soluble organic carbon (WSOC) are identified from aerosol particle samples collected with a ten-stage impactor. An iterative algorithm is developed to evaluate the hygroscopicity parameter κ from the measured chemical composition of particles. During the HaChi summer campaign, almost half of the mass concentration of particles between 150 nm and 1 μm is contributed by inorganic species. Organic matter (OM) is abundant in ultrafine particles, and 77% of the particulate mass with diameter (Dp) of around 30 nm is composed of OM. A large fraction of coarse particle mass is undetermined and is assumed to be insoluble mineral dust and liquid water. The campaign's average size distribution of κ values shows three distinct modes: a less hygroscopic mode (Dp < 150 nm) with κ slightly above 0.2, a highly hygroscopic mode (150 nm < Dp < 1 μm) with κ greater than 0.3 and a nearly hydrophobic mode (Dp > 1 μm) with κ of about 0.1. The peak of the κ curve appears around 450 nm with a maximum value of 0.35. The derived κ values are consistent with results measured with a high humidity tandem differential mobility analyzer within the size range of 50–250 nm. Inorganics are the predominant species contributing to particle hygroscopicity, especially for particles between 150 nm and 1 μm. For example, NH4NO3, H2SO4, NH4HSO4 and (NH4)2SO4 account for nearly 90% of κ for particles of around 900 nm. For ultrafine particles, WSOC plays a critical role in particle hygroscopicity due to the predominant mass fraction of OM in ultrafine particles. WSOC for particles of around 30 nm contribute 52% of κ. Aerosol hygroscopicity is related to synoptic transport patterns. When southerly wind dominates, particles are more hygroscopic; when northerly wind dominates, particles are less hygroscopic. Aerosol hygroscopicity also has a diurnal variation, which can be explained by the diurnal evolution of planetary boundary layer, photochemical aging processes during daytime and enhanced black carbon emission at night. κ is highly correlated with mass fractions of SO42−, NO3− and NH4+ for all sampled particles as well as with the mass fraction of WSOC for particles of less than 100 nm. A parameterization scheme for κ is developed using mass fractions of SO42−, NO3−, NH4+ and WSOC due to their high correlations with κ, and κ calculated from the parameterization agrees well with κ derived from the particle's chemical composition. Further analysis shows that the parameterization scheme is applicable to other aerosol studies in China.
- ItemFormation and growth of nucleated particles into cloud condensation nuclei: Model-measurement comparison(München : European Geopyhsical Union, 2013) Westervelt, D.M.; Pierce, J.R.; Riipinen, I.; Trivitayanurak, W.; Hamed, A.; Kulmala, M.; Laaksonen, A.; Decesari, S.; Adams, P.J.Aerosol nucleation occurs frequently in the atmosphere and is an important source of particle number. Observations suggest that nucleated particles are capable of growing to sufficiently large sizes that they act as cloud condensation nuclei (CCN), but some global models have reported that CCN concentrations are only modestly sensitive to large changes in nucleation rates. Here we present a novel approach for using long-term size distribution observations to evaluate a global aerosol model's ability to predict formation rates of CCN from nucleation and growth events. We derive from observations at five locations nucleation-relevant metrics such as nucleation rate of particles at diameter of 3 nm (J3), diameter growth rate (GR), particle survival probability (SP), condensation and coagulation sinks, and CCN formation rate (J100). These quantities are also derived for a global microphysical model, GEOS-Chem-TOMAS, and compared to the observations on a daily basis. Using GEOS-Chem-TOMAS, we simulate nucleation events predicted by ternary (with a 10−5 tuning factor) or activation nucleation over one year and find that the model slightly understates the observed annual-average CCN formation mostly due to bias in the nucleation rate predictions, but by no more than 50% in the ternary simulations. At the two locations expected to be most impacted by large-scale regional nucleation, Hyytiälä and San Pietro Capofiume, predicted annual-average CCN formation rates are within 34 and 2% of the observations, respectively. Model-predicted annual-average growth rates are within 25% across all sites but also show a slight tendency to underestimate the observations, at least in the ternary nucleation simulations. On days that the growing nucleation mode reaches 100 nm, median single-day survival probabilities to 100 nm for the model and measurements range from less than 1–6% across the five locations we considered; however, this does not include particles that may eventually grow to 100 nm after the first day. This detailed exploration of new particle formation and growth dynamics adds support to the use of global models as tools for assessing the contribution of microphysical processes such as nucleation to the total number and CCN budget.