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- ItemNumber size distributions and seasonality of submicron particles in Europe 2008–2009(München : European Geopyhsical Union, 2011) Asmi, A.; Wiedensohler, A.; Laj, P.; Fjaeraa, A.-M.; Sellegri, K.; Birmili, W.; Weingartner, E.; Baltensperger, U.; Zdimal, V.; Zikova, N.; Putaud, J.-P.; Marinoni, A.; Tunved, P.; Hansson, H.-C.; Fiebig, M.; Kivekäs, N.; Lihavainen, H.; Asmi, E.; Ulevicius, V.; Aalto, P.P.; Swietlicki, E.; Kristensson, A.; Mihalopoulos, N.; Kalivitis, N.; Kalapov, I.; Kiss, G.; de Leeuw, G.; Henzing, B.; Harrison, R.M.; Beddows, D.; O'Dowd, C.; Jennings, S.G.; Flentje, H.; Weinhold, K.; Meinhardt, F.; Ries, L.; Kulmala, M.Two years of harmonized aerosol number size distribution data from 24 European field monitoring sites have been analysed. The results give a comprehensive overview of the European near surface aerosol particle number concentrations and number size distributions between 30 and 500 nm of dry particle diameter. Spatial and temporal distribution of aerosols in the particle sizes most important for climate applications are presented. We also analyse the annual, weekly and diurnal cycles of the aerosol number concentrations, provide log-normal fitting parameters for median number size distributions, and give guidance notes for data users. Emphasis is placed on the usability of results within the aerosol modelling community. We also show that the aerosol number concentrations of Aitken and accumulation mode particles (with 100 nm dry diameter as a cut-off between modes) are related, although there is significant variation in the ratios of the modal number concentrations. Different aerosol and station types are distinguished from this data and this methodology has potential for further categorization of stations aerosol number size distribution types. The European submicron aerosol was divided into characteristic types: Central European aerosol, characterized by single mode median size distributions, unimodal number concentration histograms and low variability in CCN-sized aerosol number concentrations; Nordic aerosol with low number concentrations, although showing pronounced seasonal variation of especially Aitken mode particles; Mountain sites (altitude over 1000 m a.s.l.) with a strong seasonal cycle in aerosol number concentrations, high variability, and very low median number concentrations. Southern and Western European regions had fewer stations, which decreases the regional coverage of these results. Aerosol number concentrations over the Britain and Ireland had very high variance and there are indications of mixed air masses from several source regions; the Mediterranean aerosol exhibit high seasonality, and a strong accumulation mode in the summer. The greatest concentrations were observed at the Ispra station in Northern Italy with high accumulation mode number concentrations in the winter. The aerosol number concentrations at the Arctic station Zeppelin in Ny-\AA lesund in Svalbard have also a strong seasonal cycle, with greater concentrations of accumulation mode particles in winter, and dominating summer Aitken mode indicating more recently formed particles. Observed particles did not show any statistically significant regional work-week or weekday related variation in number concentrations studied. Analysis products are made for open-access to the research community, available in a freely accessible internet site. The results give to the modelling community a reliable, easy-to-use and freely available comparison dataset of aerosol size distributions.
- ItemEvaluation on the role of sulfuric acid in the mechanisms of new particle formation for Beijing case(München : European Geopyhsical Union, 2011) Wang, Z.B.; Hu, M.; Yue, D.L.; Zheng, J.; Zhang, R.Y.; Wiedensohler, A.; Wu, Z.J.; Nieminen, T.; Boy, M.New particle formation (NPF) is considered as an important mechanism for gas-to-particle transformation, and gaseous sulfuric acid is believed as a crucial precursor. Up to now few field-based studies on nucleation mechanisms and the role of sulfuric acid were conducted in China. In this study, simultaneously measurements of particle number size distributions and gaseous sulfuric acid concentrations were performed from July to September in 2008. Totally, 22 new particle formation events were observed during the entire 85 campaign days. The results show that in the case of both higher source and sink values, the result of the competition between source and sink is more likely the key limiting factor to determine the observation of NPF events in Beijing. The concentrations of gaseous sulfuric acid show good correlations with freshly nucleated particles (N3-6 and formation rates (J3 and J1.5. The power-law relationship between H2SO4 concentration and N3-6 or J is adopted to explore the nucleation mechanism. The exponents are showed a great range (from 1 to 7). More than half of the NPF events exhibit an exponent larger than 2.5. For these cases, the thermodynamic process works better than the activation or kinetic nucleation theories to explain the nucleation events in urban atmosphere of Beijing.
- ItemFirst long-term study of particle number size distributions and new particle formation events of regional aerosol in the North China Plain(München : European Geopyhsical Union, 2011) Shen, X.J.; Sun, J.Y.; Zhang, Y.M.; Wehner, B.; Nowak, A.; Tuch, T.; Zhang, X.C.; Wang, T.T.; Zhou, H.G.; Zhang, X.L.; Dong, F.; Birmili, W.; Wiedensohler, A.Atmospheric particle number size distributions (size range 0.003–10 μm) were measured between March 2008 and August 2009 at Shangdianzi (SDZ), a rural research station in the North China Plain. These measurements were made in an attempt to better characterize the tropospheric background aerosol in Northern China. The mean particle number concentrations of the total particle, as well as the nucleation, Aitken, accumulation and coarse mode were determined to be 1.2 ± 0.9 × 104, 3.6 ± 7.9 × 103, 4.4 ± 3.4 × 103, 3.5 ± 2.8 × 103 and 2 ± 3 cm−3, respectively. A general finding was that the particle number concentration was higher during spring compared to the other seasons. The air mass origin had an important effect on the particle number concentration and new particle formation events. Air masses from northwest (i.e. inner Asia) favored the new particle formation events, while air masses from southeast showed the highest particle mass concentration. Significant diurnal variations in particle number were observed, which could be linked to new particle formation events, i.e. gas-to-particle conversion. During particle formation events, the number concentration of the nucleation mode rose up to maximum value of 104 cm−3. New particle formation events were observed on 36% of the effective measurement days. The formation rate ranged from 0.7 to 72.7 cm−3 s−1, with a mean value of 8.0 cm−3 s−1. The value of the nucleation mode growth rate was in the range of 0.3–14.5 nm h−1, with a mean value of 4.3 nm h−1. It was an essential observation that on many occasions the nucleation mode was able to grow into the size of cloud condensation nuclei (CCN) within a matter of several hours. Furthermore, the new particle formation was regularly followed by a measurable increase in particle mass concentration and extinction coefficient, indicative of a high abundance of condensable vapors in the atmosphere under study.
- ItemPrimary versus secondary contributions to particle number concentrations in the European boundary layer(München : European Geopyhsical Union, 2011) Reddington, C.L.; Carslaw, K.S.; Spracklen, D.V.; Frontoso, M.G.; Collins, L.; Merikanto, J.; Minikin, A.; Hamburger, T.; Coe, H.; Kulmala, M.; Aalto, P.; Flentje, H.; Plass-Dülmer, C.; Birmili, W.; Wiedensohler, A.; Wehner, B.; Tuch, T.; Sonntag, A.; O'Dowd, C.D.; Jennings, S.G.; Dupuy, R.; Baltensperger, U.; Weingartner, E.; Hansson, H.-C.; Tunved, P.; Laj, P.; Sellegri, K.; Boulon, J.; Putaud, J.-P.; Gruening, C.; Swietlicki, E.; Roldin, P.; Henzing, J.S.; Moerman, M.; Mihalopoulos, N.; Kouvarakis, G.; ŽdÃmal, V.; ZÃková, N.; Marinoni, A.; Bonasoni, P.; Duchi, R.It is important to understand the relative contribution of primary and secondary particles to regional and global aerosol so that models can attribute aerosol radiative forcing to different sources. In large-scale models, there is considerable uncertainty associated with treatments of particle formation (nucleation) in the boundary layer (BL) and in the size distribution of emitted primary particles, leading to uncertainties in predicted cloud condensation nuclei (CCN) concentrations. Here we quantify how primary particle emissions and secondary particle formation influence size-resolved particle number concentrations in the BL using a global aerosol microphysics model and aircraft and ground site observations made during the May 2008 campaign of the European Integrated Project on Aerosol Cloud Climate Air Quality Interactions (EUCAARI). We tested four different parameterisations for BL nucleation and two assumptions for the emission size distribution of anthropogenic and wildfire carbonaceous particles. When we emit carbonaceous particles at small sizes (as recommended by the Aerosol Intercomparison project, AEROCOM), the spatial distributions of campaign-mean number concentrations of particles with diameter >50 nm (N50) and >100 nm (N100) were well captured by the model (R2≥0.8) and the normalised mean bias (NMB) was also small (−18% for N50 and −1% for N100). Emission of carbonaceous particles at larger sizes, which we consider to be more realistic for low spatial resolution global models, results in equally good correlation but larger bias (R2≥0.8, NMB = −52% and −29%), which could be partly but not entirely compensated by BL nucleation. Within the uncertainty of the observations and accounting for the uncertainty in the size of emitted primary particles, BL nucleation makes a statistically significant contribution to CCN-sized particles at less than a quarter of the ground sites. Our results show that a major source of uncertainty in CCN-sized particles in polluted European air is the emitted size of primary carbonaceous particles. New information is required not just from direct observations, but also to determine the "effective emission size" and composition of primary particles appropriate for different resolution models.
- ItemOn the sub-micron aerosol size distribution in a coastal-rural site at El Arenosillo Station (SW – Spain)(München : European Geopyhsical Union, 2011) Sorribas, M.; de la Morena, B.A.; Wehner, B.; López, J.F.; Prats, N.; Mogo, S.; Wiedensohler, A.; Cachorro, V.E.This study focuses on the analysis of the sub-micron aerosol characteristics at El Arenosillo Station, a rural and coastal environment in South-western Spain between 1 August 2004 and 31 July 2006 (594 days). The mean total concentration (NT) was 8660 cm−3 and the mean concentrations in the nucleation (NNUC), Aitken (NAIT) and accumulation (NACC) particle size ranges were 2830 cm−3, 4110 cm−3 and 1720 cm−3, respectively. Median size distribution was characterised by a single-modal fit, with a geometric diameter, median number concentration and geometric standard deviation of 60 nm, 5390 cm−3 and 2.31, respectively. Characterisation of primary emissions, secondary particle formation, changes to meteorology and long-term transport has been necessary to understand the seasonal and annual variability of the total and modal particle concentration. Number concentrations exhibited a diurnal pattern with maximum concentrations around noon. This was governed by the concentrations of the nucleation and Aitken modes during the warm seasons and only by the nucleation mode during the cold seasons. Similar monthly mean total concentrations were observed throughout the year due to a clear inverse variation between the monthly mean NNUC and NACC. It was related to the impact of desert dust and continental air masses on the monthly mean particle levels. These air masses were associated with high values of NACC which suppressed the new particle formation (decreasing NNUC). Each day was classified according to a land breeze flow or a synoptic pattern influence. The median size distribution for desert dust and continental aerosol was dominated by the Aitken and accumulation modes, and marine air masses were dominated by the nucleation and Aitken modes. Particles moved offshore due to the land breeze and had an impact on the particle burden at noon, especially when the wind was blowing from the NW sector in the morning during summer time. This increased NNUC and NAIT by factors of 3.1 and 2.4, respectively. Nucleation events with the typical "banana" shape were characterised by a mean particle nucleation rate of 0.74 cm−3 s−1, a mean growth rate of 1.96 nm h−1 and a mean total duration of 9.25 h (starting at 10:55 GMT and ending at 20:10 GMT). They were observed for 48 days. Other nucleation events were identified as those produced by the emissions from the industrial areas located at a distance of 35 km. They were observed for 42 days. Both nucleation events were strongly linked to the marine air mass origin.
- ItemSize-resolved and bulk activation properties of aerosols in the North China Plain(München : European Geopyhsical Union, 2011) Deng, Z.Z.; Zhao, C.S.; Ma, N.; Liu, P.F.; Ran, L.; Xu, W.Y.; Chen, J.; Liang, Z.; Liang, S.; Huang, M.Y.; Ma, X.C.; Zhang, Q.; Quan, J.N.; Yan, P.; Henning, S.; Mildenberger, K.; Sommerhage, E.; Schäfer, M.; Stratmann, F.; Wiedensohler, A.Size-resolved and bulk activation properties of aerosols were measured at a regional/suburban site in the North China Plain (NCP), which is occasionally heavily polluted by anthropogenic aerosol particles and gases. A Cloud Condensation Nuclei (CCN) closure study is conducted with bulk CCN number concentration (NCCN) and calculated CCN number concentration based on the aerosol number size distribution and size-resolved activation properties. The observed CCN number concentration (NCCN-obs) are higher than those observed in other locations than China, with average NCCN-obs of roughly 2000, 3000, 6000, 10 000 and 13 000 cm−3 at supersaturations of 0.056, 0.083, 0.17, 0.35 and 0.70%, respectively. An inferred critical dry diameter (Dm) is calculated based on the NCCN-obs and aerosol number size distribution assuming homogeneous chemical composition. The inferred cut-off diameters are in the ranges of 190–280, 160–260, 95–180, 65–120 and 50–100 nm at supersaturations of 0.056, 0.083, 0.17, 0.35 and 0.7%, with their mean values 230.1, 198.4, 128.4, 86.4 and 69.2 nm, respectively. Size-resolved activation measurements show that most of the 300 nm particles are activated at the investigated supersaturations, while almost no particles of 30 nm are activated even at the highest supersaturation of 0.72%. The activation ratio increases with increasing supersaturation and particle size. The slopes of the activation curves for ambient aerosols are not as steep as those observed in calibrations with ammonium sulfate suggesting that the observed aerosols is an external mixture of more hygroscopic and hydrophobic particles. The calculated CCN number concentrations (NCCN-calc) based on the size-resolved activation ratio and aerosol number size distribution correlate well with the NCCN-obs, and show an average overestimation of 19%. Sensitivity studies of the CCN closure show that the NCCN at each supersaturation is well predicted with the campaign average of size-resolved activation curves. These results indicate that the aerosol number size distribution is critical in the prediction of possible CCN. The CCN number concentration can be reliably estimated using time-averaged, size-resolved activation efficiencies without accounting for the temporal variations.
- ItemChemical mass balance of 300 °c non-volatile particles at the tropospheric research site Melpitz, Germany(München : European Geopyhsical Union, 2014) Poulain, L.; Birmili, W.; Canonaco, F.; Crippa, M.; Wu, Z.J.; Nordmann, S.; Wiedensohler, A.; Held, A.; Spindler, G.; Prévôt, A.S.H.; Wiedensohler, A.; Herrmann, H.In the fine-particle mode (aerodynamic diameter < 1 μm) non-volatile material has been associated with black carbon (BC) and low-volatile organics and, to a lesser extent, with sea salt and mineral dust. This work analyzes non-volatile particles at the tropospheric research station Melpitz (Germany), combining experimental methods such as a mobility particle-size spectrometer (3–800 nm), a thermodenuder operating at 300 °C, a multi-angle absorption photometer (MAAP), and an aerosol mass spectrometer (AMS). The data were collected during two atmospheric field experiments in May–June 2008 as well as February–March 2009. As a basic result, we detected average non-volatile particle–volume fractions of 11 ± 3% (2008) and 17 ± 8% (2009). In both periods, BC was in close linear correlation with the non-volatile fraction, but not sufficient to quantitatively explain the non-volatile particle mass concentration. Based on the assumption that BC is not altered by the heating process, the non-volatile particle mass fraction could be explained by the sum of black carbon (47% in summer, 59% in winter) and a non-volatile organic contribution estimated as part of the low-volatility oxygenated organic aerosol (LV-OOA) (53% in summer, 41% in winter); the latter was identified from AMS data by factor analysis. Our results suggest that LV-OOA was more volatile in summer (May–June 2008) than in winter (February–March 2009) which was linked to a difference in oxidation levels (lower in summer). Although carbonaceous compounds dominated the sub-μm non-volatile particle mass fraction most of the time, a cross-sensitivity to partially volatile aerosol particles of maritime origin could be seen. These marine particles could be distinguished, however from the carbonaceous particles by a characteristic particle volume–size distribution. The paper discusses the uncertainty of the volatility measurements and outlines the possible merits of volatility analysis as part of continuous atmospheric aerosol measurements.
- ItemAnalysis of number size distributions of tropical free tropospheric aerosol particles observed at Pico Espejo (4765 m a.s.l.), Venezuela(München : European Geopyhsical Union, 2011) Schmeissner, T.; Krejci, R.; Ström, J.; Birmili, W.; Wiedensohler, A.; Hochschild, G.; Gross, J.; Hoffmann, P.; Calderon, S.The first long-term measurements of aerosol number and size distributions in South-American tropical free troposphere (FT) were performed from March 2007 until March 2009. The measurements took place at the high altitude Atmospheric Research Station Alexander von Humboldt. The station is located on top of the Sierra Nevada mountain ridge at 4765 m a.s.l. nearby the city of Mérida, Venezuela. Aerosol size distribution and number concentration data was obtained with a custom-built Differential Mobility Particle Sizer (DMPS) system and a Condensational Particle Counter (CPC). The analysis of the annual and diurnal variability of the tropical FT aerosol focused mainly on possible links to the atmospheric general circulation in the tropics. Considerable annual and diurnal cycles of the particle number concentration were observed. Highest total particle number concentrations were measured during the dry season (January–March, 519 ± 613 cm−3), lowest during the wet season (July–September, 318 ± 194 cm−3). The more humid FT (relative humidity (RH) range 50–95 %) contained generally higher aerosol particle number concentrations (573 ± 768 cm−3 during dry season, 320 ± 195 cm−3 during wet season) than the dry FT (RH < 50 %, 454 ± 332 cm−3 during dry season, 275 ± 172 cm−3 during wet season), indicating the importance of convection for aerosol distributions in the tropical FT. The diurnal cycle in the variability of the particle number concentration was mainly driven by local orography.
- ItemCharacteristics of regional new particle formation in urban and regional background environments in the North China Plain(München : European Geopyhsical Union, 2013) Wang, Z.B.; Hu, M.; Sun, J.Y.; Wu, Z.J.; Yue, D.L.; Shen, X.J.; Zhang, Y.M.; Pei, X.Y.; Cheng, Y.F.; Wiedensohler, A.Long-term measurements of particle number size distributions were carried out both at an urban background site (Peking University, PKU) and a regional Global Atmospheric Watch station (Shangdianzi, SDZ) from March to November in 2008. In total, 52 new particle formation (NPF) events were observed simultaneously at both sites, indicating that this is a regional phenomenon in the North China Plain. On average, the mean condensation sink value before the nucleation events started was 0.025 s−1 in the urban environment, which was 1.6 times higher than that at regional site. However, higher particle formation and growth rates were observed at PKU (10.8 cm−3 s−1 and 5.2 nm h−1) compared with those at SDZ (4.9 cm−3 s−1 and 4.0 nm h−1). These results implied that precursors were much more abundant in the polluted urban environment. Different from the observations in cleaner environments, the background conditions of the observed particle homogeneous nucleation events in the North China Plain could be characterized as the co-existing of a stronger source of precursor gases and a higher condensational sink of pre-existing aerosol particles. Secondary aerosol formation following nucleation events results in an increase of particle mass concentration, particle light scattering coefficient, and cloud condensation nuclei (CCN) number concentration, with consequences on visibility, radiative effects, and air quality. Typical regional NPF events with significant particle nucleation rates and subsequent particle growth over a sufficiently long time period at both sites were chosen to investigate the influence of NPF on the number concentration of "potential" CCN. As a result, the NPF and the subsequent condensable growth increased the CCN number concentration in the North China Plain by factors in the range from 5.6 to 8.7. Moreover, the potential contribution of anthropogenic emissions to the CCN number concentration was more than 50%, to which more attention should be drawn in regional and global climate modeling, especially in the polluted urban areas.
- ItemCloud condensation nuclei in polluted air and biomass burning smoke near the mega-city Guangzhou, China – Part 2: Size-resolved aerosol chemical composition, diurnal cycles, and externally mixed weakly CCN-active soot particles(München : European Geopyhsical Union, 2011) Rose, D.; Gunthe, S.S.; Su, H.; Garland, R.M.; Yang, H.; Berghof, M.; Cheng, Y.F.; Wehner, B.; Achtert, P.; Nowak, A.; Wiedensohler, A.; Takegawa, N.; Kondo, Y.; Hu, M.; Zhang, Y.; Andreae, M.O.; Pöschl, U.Size-resolved chemical composition, mixing state, and cloud condensation nucleus (CCN) activity of aerosol particles in polluted mega-city air and biomass burning smoke were measured during the PRIDE-PRD2006 campaign near Guangzhou, China, using an aerosol mass spectrometer (AMS), a volatility tandem differential mobility analyzer (VTDMA), and a continuous-flow CCN counter (DMT-CCNC). The size-dependence and temporal variations of the effective average hygroscopicity parameter for CCN-active particles (κa) could be parameterized as a function of organic and inorganic mass fractions (forg, finorg) determined by the AMS: κa,p=κorg·forg + κinorg·finorg. The characteristic κ values of organic and inorganic components were similar to those observed in other continental regions of the world: κorg≈0.1 and κinorg≈0.6. The campaign average κa values increased with particle size from ~0.25 at ~50 nm to ~0.4 at ~200 nm, while forg decreased with particle size. At ~50 nm, forg was on average 60% and increased to almost 100% during a biomass burning event. The VTDMA results and complementary aerosol optical data suggest that the large fractions of CCN-inactive particles observed at low supersaturations (up to 60% at S≤0.27%) were externally mixed weakly CCN-active soot particles with low volatility (diameter reduction <5% at 300 °C) and effective hygroscopicity parameters around κLV≈0.01. A proxy for the effective average hygroscopicity of the total ensemble of CCN-active particles including weakly CCN-active particles (κt) could be parameterized as a function of κa,p and the number fraction of low volatility particles determined by VTDMA (φLV): κt,p=κa,p−φLV·(κa,p−κLV). Based on κ values derived from AMS and VTDMA data, the observed CCN number concentrations (NCCN,S≈102–104 cm−3 at S = 0.068–0.47%) could be efficiently predicted from the measured particle number size distribution. The mean relative deviations between observed and predicted CCN concentrations were ~10% when using κt,p, and they increased to ~20% when using only κa,p. The mean relative deviations were not higher (~20%) when using an approximate continental average value of κ≈0.3, although the constant κ value cannot account for the observed temporal variations in particle composition and mixing state (diurnal cycles and biomass burning events). Overall, the results confirm that on a global and climate modeling scale an average value of κ≈0.3 can be used for approximate predictions of CCN number concentrations in continental boundary layer air when aerosol size distribution data are available without information about chemical composition. Bulk or size-resolved data on aerosol chemical composition enable improved CCN predictions resolving regional and temporal variations, but the composition data need to be highly accurate and complemented by information about particle mixing state to achieve high precision (relative deviations <20%).