2018, Chen, Jie, Wu, Zhijun, Augustin-Bauditz, Stefanie, Grawe, Sarah, Hartmann, Markus, Pei, Xiangyu, Liu, Zirui, Ji, Dongsheng, Wex, Heike

Exceedingly high levels of PM2.5 with complex chemical composition occur frequently in China. It has been speculated whether anthropogenic PM2.5 may significantly contribute to ice-nucleating particles (INP). However, few studies have focused on the ice-nucleating properties of urban particles. In this work, two ice-nucleating droplet arrays have been used to determine the atmospheric number concentration of INP (NINP) in the range from -6 to -25 °C in Beijing. No correlations between NINP and either PM2.5 or black carbon mass concentrations were found, although both varied by more than a factor of 30 during the sampling period. Similarly, there were no correlations between NINP and either total particle number concentration or number concentrations for particles with diameters > 500 nm. Furthermore, there was no clear difference between day and night samples. All these results indicate that Beijing air pollution did not increase or decrease INP concentrations in the examined temperature range above values observed in nonurban areas; hence, the background INP concentrations might not be anthropogenically influenced as far as urban air pollution is concerned, at least in the examined temperature range.

2017, Martinsson, Bengt G., Friberg, Johan, Sandvik, Oscar S., Hermann, Markus, van Velthoven, Peter F. J., Zahn, Andreas

This study is based on fine-mode aerosol samples collected in the upper troposphere (UT) and the lowermost stratosphere (LMS) of the Northern Hemisphere extratropics during monthly intercontinental flights at 8.8-12 km altitude of the IAGOS-CARIBIC platform in the time period 1999-2014. The samples were analyzed for a large number of chemical elements using the accelerator-based methods PIXE (particle-induced X-ray emission) and PESA (particle elastic scattering analysis). Here the particulate sulfur concentrations, obtained by PIXE analysis, are investigated. In addition, the satellite-borne lidar aboard CALIPSO is used to study the stratospheric aerosol load. A steep gradient in particulate sulfur concentration extends several kilometers into the LMS, as a result of increasing dilution towards the tropopause of stratospheric, particulate sulfur-rich air. The stratospheric air is diluted with tropospheric air, forming the extratropical transition layer (ExTL). Observed concentrations are related to the distance to the dynamical tropopause. A linear regression methodology handled seasonal variation and impact from volcanism. This was used to convert each data point into stand-alone estimates of a concentration profile and column concentration of particulate sulfur in a 3 km altitude band above the tropopause. We find distinct responses to volcanic eruptions, and that this layer in the LMS has a significant contribution to the stratospheric aerosol optical depth and thus to its radiative forcing. Further, the origin of UT particulate sulfur shows strong seasonal variation. We find that tropospheric sources dominate during the fall as a result of downward transport of the Asian tropopause aerosol layer (ATAL) formed in the Asian monsoon, whereas transport down from the Junge layer is the main source of UT particulate sulfur in the first half of the year. In this latter part of the year, the stratosphere is the clearly dominating source of particulate sulfur in the UT during times of volcanic influence and under background conditions.

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.

2018, Zhu, Yanhong, Yang, Lingxiao, Chen, Jianmin, Kawamura, Kimitaka, Sato, Mamiko, Tilgner, Andreas, van Pinxteren, Dominik, Chen, Ying, Xue, Likun, Wang, Xinfeng, Simpson, Isobel J., Herrmann, Hartmut, Blake, Donald R., Wang, Wenxing

Fine particulate matter (PM2.5) samples collected at Mount (Mt.) Tai in the North China Plain during summer 2014 were analyzed for dicarboxylic acids and related compounds (oxocarboxylic acids and α-dicarbonyls) (DCRCs). The total concentration of DCRCs was 1050±580 and 1040±490ng m-3 during the day and night, respectively. Although these concentrations were about 2 times lower than similar measurements in 2006, the concentrations reported here were about 1-13 times higher than previous measurements in other major cities in the world. Molecular distributions of DCRCs revealed that oxalic acid (C2) was the dominant species (50%), followed by succinic acid (C4) (12%) and malonic acid (C3) (8%). WRF modeling revealed that Mt. Tai was mostly in the free troposphere during the campaign and long-range transport was a major factor governing the distributions of the measured compounds at Mt. Tai. A majority of the samples (79%) had comparable concentrations during the day and night, with their day-night concentration ratios between 0.9 and 1.1. Multi-day transport was considered an important reason for the similar concentrations. Correlation analyses of DCRCs and their gas precursors and between C2 and sulfate indicated precursor emissions and aqueous-phase oxidations during long-range transport also likely play an important role, especially during the night. Source identification indicated that anthropogenic activities followed by photochemical aging accounted for about 60% of the total variance and were the dominant source at Mt. Tai. However, biomass burning was only important during the first half of the measurement period. Measurements of potassium (K+) and DCRCs were about 2 times higher than those from the second half of the measurement period. The concentration of levoglucosan, a biomass burning tracer, decreased by about 80% between 2006 and 2014, indicating that biomass burning may have decreased between 2006 and 2014.

2018, Größ, Johannes, Hamed, Amar, Sonntag, André, Spindler, Gerald, Manninen, Hanna Elina, Nieminen, Tuomo, Kulmala, Markku, Hõrrak, Urmas, Plass-Dülmer, Christian, Wiedensohler, Alfred, Birmili, Wolfram

This paper revisits the atmospheric new particle formation (NPF) process in the polluted Central European troposphere, focusing on the connection with gas-phase precursors and meteorological parameters. Observations were made at the research station Melpitz (former East Germany) between 2008 and 2011 involving a neutral cluster and air ion spectrometer (NAIS). Particle formation events were classified by a new automated method based on the convolution integral of particle number concentration in the diameter interval 2-20 nm. To study the relevance of gaseous sulfuric acid as a precursor for nucleation, a proxy was derived on the basis of direct measurements during a 1-month campaign in May 2008. As a major result, the number concentration of freshly produced particles correlated significantly with the concentration of sulfur dioxide as the main precursor of sulfuric acid. The condensation sink, a factor potentially inhibiting NPF events, played a subordinate role only. The same held for experimentally determined ammonia concentrations. The analysis of meteorological parameters confirmed the absolute need for solar radiation to induce NPF events and demonstrated the presence of significant turbulence during those events. Due to its tight correlation with solar radiation, however, an independent effect of turbulence for NPF could not be established. Based on the diurnal evolution of aerosol, gas-phase, and meteorological parameters near the ground, we further conclude that the particle formation process is likely to start in elevated parts of the boundary layer rather than near ground level.

2018, Nieminen, Tuomo, Kerminen, Veli-Matti, Petäjä, Tuukka, Aalto, Pasi P., Arshinov, Mikhail, Asmi, Eija, Baltensperger, Urs, Beddows, David C. S., Beukes, Johan Paul, Collins, Don, Ding, Aijun, Harrison, Roy M., Henzing, Bas, Hooda, Rakesh, Hu, Min, Hõrrak, Urmas, Kivekäs, Niku, Komsaare, Kaupo, Krejci, Radovan, Kristensson, Adam, Laakso, Lauri, Laaksonen, Ari, Leaitch, W. Richard, Lihavainen, Heikki, Mihalopoulos, Nikolaos, Németh, Zoltán, Nie, Wei, O'Dowd, Colin, Salma, Imre, Sellegri, Karine, Svenningsson, Birgitta, Swietlicki, Erik, Tunved, Peter, Ulevicius, Vidmantas, Vakkari, Ville, Vana, Marko, Wiedensohler, Alfred, Wu, Zhijun, Virtanen, Annele, Kulmala, Markku

Atmospheric new particle formation (NPF) is an important phenomenon in terms of global particle number concentrations. Here we investigated the frequency of NPF, formation rates of 10 nm particles, and growth rates in the size range of 10–25 nm using at least 1 year of aerosol number size-distribution observations at 36 different locations around the world. The majority of these measurement sites are in the Northern Hemisphere. We found that the NPF frequency has a strong seasonal variability. At the measurement sites analyzed in this study, NPF occurs most frequently in March–May (on about 30 % of the days) and least frequently in December-February (about 10 % of the days). The median formation rate of 10 nm particles varies by about 3 orders of magnitude (0.01–10 cm−3 s−1) and the growth rate by about an order of magnitude (1–10 nm h−1). The smallest values of both formation and growth rates were observed at polar sites and the largest ones in urban environments or anthropogenically influenced rural sites. The correlation between the NPF event frequency and the particle formation and growth rate was at best moderate among the different measurement sites, as well as among the sites belonging to a certain environmental regime. For a better understanding of atmospheric NPF and its regional importance, we would need more observational data from different urban areas in practically all parts of the world, from additional remote and rural locations in North America, Asia, and most of the Southern Hemisphere (especially Australia), from polar areas, and from at least a few locations over the oceans.

2018, Papagiannopoulos, Nikolaos, Mona, Lucia, Amodeo, Aldo, D'Amico, Giuseppe, Gumà Claramunt, Pilar, Pappalardo, Gelsomina, Alados-Arboledas, Lucas, Guerrero-Rascado, Juan Luís, Amiridis, Vassilis, Kokkalis, Panagiotis, Apituley, Arnoud, Baars, Holger, Schwarz, Anja, Wandinger, Ulla, Binietoglou, Ioannis, Nicolae, Doina, Bortoli, Daniele, Comerón, Adolfo, Rodríguez-Gómez, Alejandro, Sicard, Michaël, Papayannis, Alex, Wiegner, Matthias

We present an automatic aerosol classification method based solely on the European Aerosol Research Lidar Network (EARLINET) intensive optical parameters with the aim of building a network-wide classification tool that could provide near-real-time aerosol typing information. The presented method depends on a supervised learning technique and makes use of the Mahalanobis distance function that relates each unclassified measurement to a predefined aerosol type. As a first step (training phase), a reference dataset is set up consisting of already classified EARLINET data. Using this dataset, we defined 8 aerosol classes: clean continental, polluted continental, dust, mixed dust, polluted dust, mixed marine, smoke, and volcanic ash. The effect of the number of aerosol classes has been explored, as well as the optimal set of intensive parameters to separate different aerosol types. Furthermore, the algorithm is trained with literature particle linear depolarization ratio values. As a second step (testing phase), we apply the method to an already classified EARLINET dataset and analyze the results of the comparison to this classified dataset. The predictive accuracy of the automatic classification varies between 59% (minimum) and 90% (maximum) from 8 to 4 aerosol classes, respectively, when evaluated against pre-classified EARLINET lidar. This indicates the potential use of the automatic classification to all network lidar data. Furthermore, the training of the algorithm with particle linear depolarization values found in the literature further improves the accuracy with values for all the aerosol classes around 80%. Additionally, the algorithm has proven to be highly versatile as it adapts to changes in the size of the training dataset and the number of aerosol classes and classifying parameters. Finally, the low computational time and demand for resources make the algorithm extremely suitable for the implementation within the single calculus chain (SCC), the EARLINET centralized processing suite.

2017, Li, Jiarong, Wang, Xinfeng, Chen, Jianmin, Zhu, Chao, Li, Weijun, Li, Chengbao, Liu, Lu, Xu, Caihong, Wen, Liang, Xue, Likun, Wang, Wenxing, Ding, Aijun, Herrmann, Hartmut

The chemical composition of 39 cloud samples and droplet size distributions in 24 cloud events were investigated at the summit of Mt. Tai from July to October 2014. Inorganic ions, organic acids, metals, HCHO, H2O2, sulfur( IV), organic carbon, and elemental carbon as well as pH and electrical conductivity were analyzed. The acidity of the cloud water significantly decreased from a reported value of pH 3.86 during 2007-2008 (Guo et al., 2012) to pH 5.87 in the present study. The concentrations of nitrate and ammonium were both increased since 2007-2008, but the overcompensation of ammonium led to an increase in the mean pH value. The microphysical properties showed that cloud droplets were smaller than 26.0 μm and most were in the range of 6.0-9.0 μm at Mt. Tai. The maximum droplet number concentration (Nd) was associated with a droplet size of 7.0 μm. High liquid water content (LWC) values could facilitate the formation of larger cloud droplets and broadened the droplet size distribution. Cloud droplets exhibited a strong interaction with atmospheric aerosols. Higher PM2.5 levels resulted in higher concentrations of water-soluble ions and smaller sizes with increased numbers of cloud droplets. The lower pH values were likely to occur at higher PM2.5 concentrations. Clouds were an important sink for soluble materials in the atmosphere. The dilution effect of cloud water should be considered when estimating concentrations of soluble components in the cloud phase.

2017, Bozzetti, Carlo, El Haddad, Imad, Salameh, Dalia, Daellenbach, Kaspar Rudolf, Fermo, Paola, Gonzalez, Raquel, Minguillón, María Cruz, Iinuma, Yoshiteru, Poulain, Laurent, Elser, Miriam, Müller, Emanuel, Slowik, Jay Gates, Jaffrezo, Jean-Luc, Baltensperger, Urs, Marchand, Nicolas, Prévôt, André Stephan Henry

We investigated the seasonal trends of OA sources affecting the air quality of Marseille (France), which is the largest harbor of the Mediterranean Sea. This was achieved by measurements of nebulized filter extracts using an aerosol mass spectrometer (offline-AMS). In total 216 PM2.5 (particulate matter with an aerodynamic diameter < 2.5 μm) filter samples were collected over 1 year from August 2011 to July 2012. These filters were used to create 54 composite samples which were analyzed by offline-AMS. The same samples were also analyzed for major water-soluble ions, metals, elemental and organic carbon (EC/OC), and organic markers, including n-alkanes, hopanes, polycyclic aromatic hydrocarbons (PAHs), lignin and cellulose pyrolysis products, and nitrocatechols. The application of positive matrix factorization (PMF) to the water-soluble AMS spectra enabled the extraction of five factors, related to hydrocarbon-like OA (HOA), cooking OA (COA), biomass burning OA (BBOA), oxygenated OA (OOA), and an industry-related OA (INDOA). Seasonal trends and relative contributions of OA sources were compared with the source apportionment of OA spectra collected from the AMS field deployment at the same station but in different years and for shorter monitoring periods (February 2011 and July 2008). Online- and offline-AMS source apportionment revealed comparable seasonal contribution of the different OA sources. Results revealed that BBOA was the dominant source during winter, representing on average 48 % of the OA, while during summer the main OA component was OOA (63 % of OA mass on average). HOA related to traffic emissions contributed on a yearly average 17 % to the OA mass, while COA was a minor source contributing 4 %. The contribution of INDOA was enhanced during winter (17 % during winter and 11 % during summer), consistent with an increased contribution from light alkanes, light PAHs (fluoranthene, pyrene, phenanthrene), and selenium, which is commonly considered as a unique coal combustion and coke production marker. Online- and offline-AMS source apportionments revealed evolving levoglucosan : BBOA ratios, which were higher during late autumn and March. A similar seasonality was observed in the ratios of cellulose combustion markers to lignin combustion markers, highlighting the contribution from cellulose-rich biomass combustion, possibly related to agricultural activities.

2018, Pandolfi, Marco, Alados-Arboledas, Lucas, Alastuey, Andrés, Andrade, Marcos, Angelov, Christo, Artiñano, Begoña, Backman, John, Baltensperger, Urs, Bonasoni, Paolo, Bukowiecki, Nicolas, Collaud Coen, Martine, Conil, Sébastien, Coz, Esther, Crenn, Vincent, Dudoitis, Vadimas, Ealo, Marina, Eleftheriadis, Kostas, Favez, Olivier, Fetfatzis, Prodromos, Fiebig, Markus, Flentje, Harald, Ginot, Patrick, Gysel, Martin, Henzing, Bas, Hoffer, Andras, Holubova Smejkalova, Adela, Kalapov, Ivo, Kalivitis, Nikos, Kouvarakis, Giorgos, Kristensson, Adam, Kulmala, Markku, Lihavainen, Heikki, Lunder, Chris, Luoma, Krista, Lyamani, Hassan, Marinoni, Angela, Mihalopoulos, Nikos, Moerman, Marcel, Nicolas, José, O'Dowd, Colin, Petäjä, Tuukka, Petit, Jean-Eudes, Pichon, Jean Marc, Prokopciuk, Nina, Putaud, Jean-Philippe, Rodríguez, Sergio, Sciare, Jean, Sellegri, Karine, Swietlicki, Erik, Titos, Gloria, Tuch, Thomas, Tunved, Peter, Ulevicius, Vidmantas, Vaishya, Aditya, Vana, Milan, Virkkula, Aki, Vratolis, Stergios, Weingartner, Ernest, Wiedensohler, Alfred, Laj, Paolo

This paper presents the light-scattering properties of atmospheric aerosol particles measured over the past decade at 28 ACTRIS observatories, which are located mainly in Europe. The data include particle light scattering (σsp) and hemispheric backscattering (σbsp) coefficients, scattering Ångström exponent (SAE), backscatter fraction (BF) and asymmetry parameter (g). An increasing gradient of σsp is observed when moving from remote environments (arctic/mountain) to regional and to urban environments. At a regional level in Europe, σsp also increases when moving from Nordic and Baltic countries and from western Europe to central/eastern Europe, whereas no clear spatial gradient is observed for other station environments. The SAE does not show a clear gradient as a function of the placement of the station. However, a west-to-east-increasing gradient is observed for both regional and mountain placements, suggesting a lower fraction of fine-mode particle in western/south-western Europe compared to central and eastern Europe, where the fine-mode particles dominate the scattering. The g does not show any clear gradient by station placement or geographical location reflecting the complex relationship of this parameter with the physical properties of the aerosol particles. Both the station placement and the geographical location are important factors affecting the intraannual variability. At mountain sites, higher σsp and SAE values are measured in the summer due to the enhanced boundary layer influence and/or new particle-formation episodes. Conversely, the lower horizontal and vertical dispersion during winter leads to higher σsp values at all low-altitude sites in central and eastern Europe compared to summer. These sites also show SAE maxima in the summer (with corresponding g minima). At all sites, both SAE and g show a strong variation with aerosol particle loading. The lowest values of g are always observed together with low σsp values, indicating a larger contribution from particles in the smaller accumulation mode. During periods of high σsp values, the variation of g is less pronounced, whereas the SAE increases or decreases, suggesting changes mostly in the coarse aerosol particle mode rather than in the fine mode. Statistically significant decreasing trends of σsp are observed at 5 out of the 13 stations included in the trend analyses. The total reductions of σsp are consistent with those reported for PM2.5 and PM10 mass concentrations over similar periods across Europe.