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- 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 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.
- ItemOn the abundance and source contributions of dicarboxylic acids in size-resolved aerosol particles at continental sites in central Europe(München : European Geopyhsical Union, 2014) van Pinxteren, D.; Neusüß, C.; Herrmann, H.Dicarboxylic acids (DCAs) are among the most abundant organic compounds observed in atmospheric aerosol particles and have been extensively studied at many places around the world. The importance of the various primary sources and secondary formation pathways discussed in the literature is often difficult to assess from field studies, though. In the present study, a large data set of size-resolved DCA concentrations from several inland sites in Germany is combined with results from a recently developed approach of statistical back-trajectory analysis and additional data. Principal component analysis is then used to reveal the most important factors governing the abundance of DCAs in different particle size ranges. The two most important sources revealed are (i) photochemical formation during intense radiation days in polluted air masses, likely occurring in the gas phase on short timescales (gasSOA), and (ii) secondary reactions in anthropogenically influenced air masses, likely occurring in the aqueous phase on longer timescales (aqSOA). While the first source strongly impacts DCA concentrations mainly in small and large particles, the second one enhances accumulation mode DCAs and is responsible for the bulk of the observed concentrations. Primary sources were found to be minor (sea salt, soil resuspension) or non-existent (biomass burning, traffic). The results can be regarded as representative for typical central European continental conditions.
- ItemSeasonal variability of Saharan desert dust and ice nucleating particles over Europe(München : European Geopyhsical Union, 2015) Hande, L.B.; Engler, C.; Hoose, C.; Tegen, I.Dust aerosols are thought to be the main contributor to atmospheric ice nucleation. While there are case studies supporting this, a climatological sense of the importance of dust to atmospheric ice nucleating particle (INP) concentrations and its seasonal variability over Europe is lacking. Here, we use a mesoscale model to estimate Saharan dust concentrations over Europe in 2008. There are large differences in median dust concentrations between seasons, with the highest concentrations and highest variability in the lower to mid-troposphere. Laboratory-based ice nucleation parameterisations are applied to these simulated dust number concentrations to calculate the potential INP resulting from immersion freezing and deposition nucleation on these dust particles. The potential INP concentrations increase exponentially with height due to decreasing temperatures in the lower and mid-troposphere. When the ice-activated fraction increases sufficiently, INP concentrations follow the dust particle concentrations. The potential INP profiles exhibit similarly large differences between seasons, with the highest concentrations in spring (median potential immersion INP concentrations nearly 105 m−3, median potential deposition INP concentrations at 120% relative humidity with respect to ice over 105 m−3), about an order of magnitude larger than those in summer. Using these results, a best-fit function is provided to estimate the potential INPs for use in limited-area models, which is representative of the normal background INP concentrations over Europe. A statistical evaluation of the results against field and laboratory measurements indicates that the INP concentrations are in close agreement with observations.
- ItemA method for detecting the presence of organic fraction in nucleation mode sized particles(München : European Geopyhsical Union, 2005) Vaattovaara, P.; Räsänen, M.; Kühn, T.; Joutsensaari, J.; Laaksonen, A.New particle formation and growth has a very important role in many climate processes. However, the overall knowlegde of the chemical composition of atmospheric nucleation mode (particle diameter, d<20 nm) and the lower end of Aitken mode particles (d≤50 nm) is still insufficient. In this work, we have applied the UFO-TDMA (ultrafine organic tandem differential mobility analyzer) method to shed light on the presence of an organic fraction in the nucleation mode size class in different atmospheric environments. The basic principle of the organic fraction detection is based on our laboratory UFO-TDMA measurements with organic and inorganic compounds. Our laboratory measurements indicate that the usefulness of the UFO-TDMA in the field experiments would arise especially from the fact that atmospherically the most relevant inorganic compounds do not grow in subsaturated ethanol vapor, when particle size is 10 nm in diameter and saturation ratio is about 86% or below it. Furthermore, internally mixed particles composed of ammonium bisulfate and sulfuric acid with sulfuric acid mass fraction ≤33% show no growth at 85% saturation ratio. In contrast, 10 nm particles composed of various oxidized organic compounds of atmospheric relevance are able to grow in those conditions. These discoveries indicate that it is possible to detect the presence of organics in atmospheric nucleation mode sized particles using the UFO-TDMA method. In the future, the UFO-TDMA is expected to be an important aid to describe the composition of atmospheric newly-formed particles.
- ItemAqueous phase oxidation of sulphur dioxide by ozone in cloud droplets(München : European Geopyhsical Union, 2016) Hoyle, C.R.; Fuchs, C.; Järvinen, E.; Saathoff, H.; Dias, A.; El Haddad, I.; Gysel, M.; Coburn, S.C.; Tröstl, J.; Bernhammer, A.-K.; Bianchi, F.; Breitenlechner, M.; Corbin, J.C.; Craven, J.; Donahue, N.M.; Duplissy, J.; Ehrhart, S.; Frege, C.; Gordon, H.; Höppel, N.; Heinritzi, M.; Kristensen, T.B.; Molteni, U.; Nichman, L.; Pinterich, T.; Prévôt, A.S.H.; Simon, M.; Slowik, J.G.; Steiner, G.; Tomé, A.; Vogel, A.L.; Volkamer, R.; Wagner, A.C.; Wagner, R.; Wexler, A.S.; Williamson, C.; Winkler, P.M.; Amorim, A.; Dommen, J.; Curtius, J.; Gallagher, M.W.; Flagan, R.C.; Hansel, A.; Kirkby, J.; Kulmala, M.; Möhler, O.; Stratmann, F.; Worsnop, D.R.; Baltensperger, U.The growth of aerosol due to the aqueous phase oxidation of sulfur dioxide by ozone was measured in laboratory-generated clouds created in the Cosmics Leaving OUtdoor Droplets (CLOUD) chamber at the European Organization for Nuclear Research (CERN). Experiments were performed at 10 and −10 °C, on acidic (sulfuric acid) and on partially to fully neutralised (ammonium sulfate) seed aerosol. Clouds were generated by performing an adiabatic expansion – pressurising the chamber to 220 hPa above atmospheric pressure, and then rapidly releasing the excess pressure, resulting in a cooling, condensation of water on the aerosol and a cloud lifetime of approximately 6 min. A model was developed to compare the observed aerosol growth with that predicted using oxidation rate constants previously measured in bulk solutions. The model captured the measured aerosol growth very well for experiments performed at 10 and −10 °C, indicating that, in contrast to some previous studies, the oxidation rates of SO2 in a dispersed aqueous system can be well represented by using accepted rate constants, based on bulk measurements. To the best of our knowledge, these are the first laboratory-based measurements of aqueous phase oxidation in a dispersed, super-cooled population of droplets. The measurements are therefore important in confirming that the extrapolation of currently accepted reaction rate constants to temperatures below 0 °C is correct.