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.

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.

2012, Wiedensohler, A., Birmili, W., Nowak, A., Sonntag, A., Weinhold, K., Merkel, M., Wehner, B., Tuch, T., Pfeifer, S., Fiebig, M., Fjäraa, A.M., Asmi, E., Sellegri, K., Depuy, R., Venzac, H., Villani, P., Laj, P., Aalto, P., Ogren, J.A., Swietlick, E., Williams, P., Roldin, P., Quincey, P., Hüglin, C., Fierz-Schmidhauser, R., Gysel, M., Weingartner, E., Riccobono, F., Santos, S., Grüning, C., Faloon, K., Beddows, D., Harrison, R., Monahan, C., Jennings, S.G., O'Dowd, C.D., Marinoni, A., Horn, H.-G., Keck, L., Jiang, J., Scheckman, J., McMurry, P.H., Deng, Z., Zhao, C.S., Moerman, M., Henzing, B., de Leeuw, G., Löschau, G., Bastian, S.

Mobility particle size spectrometers often referred to as DMPS (Differential Mobility Particle Sizers) or SMPS (Scanning Mobility Particle Sizers) have found a wide range of applications in atmospheric aerosol research. However, comparability of measurements conducted world-wide is hampered by lack of generally accepted technical standards and guidelines with respect to the instrumental set-up, measurement mode, data evaluation as well as quality control. Technical standards were developed for a minimum requirement of mobility size spectrometry to perform long-term atmospheric aerosol measurements. Technical recommendations include continuous monitoring of flow rates, temperature, pressure, and relative humidity for the sheath and sample air in the differential mobility analyzer. We compared commercial and custom-made inversion routines to calculate the particle number size distributions from the measured electrical mobility distribution. All inversion routines are comparable within few per cent uncertainty for a given set of raw data. Furthermore, this work summarizes the results from several instrument intercomparison workshops conducted within the European infrastructure project EUSAAR (European Supersites for Atmospheric Aerosol Research) and ACTRIS (Aerosols, Clouds, and Trace gases Research InfraStructure Network) to determine present uncertainties especially of custom-built mobility particle size spectrometers. Under controlled laboratory conditions, the particle number size distributions from 20 to 200 nm determined by mobility particle size spectrometers of different design are within an uncertainty range of around ±10% after correcting internal particle losses, while below and above this size range the discrepancies increased. For particles larger than 200 nm, the uncertainty range increased to 30%, which could not be explained. The network reference mobility spectrometers with identical design agreed within ±4% in the peak particle number concentration when all settings were done carefully. The consistency of these reference instruments to the total particle number concentration was demonstrated to be less than 5%. Additionally, a new data structure for particle number size distributions was introduced to store and disseminate the data at EMEP (European Monitoring and Evaluation Program). This structure contains three levels: raw data, processed data, and final particle size distributions. Importantly, we recommend reporting raw measurements including all relevant instrument parameters as well as a complete documentation on all data transformation and correction steps. These technical and data structure standards aim to enhance the quality of long-term size distribution measurements, their comparability between different networks and sites, and their transparency and traceability back to raw data.

2014, Beddows, D.C.S., Dall'Osto, M., Harrison, R.M., Kulmala, M., Asmi, A., Wiedensohler, A., Laj, P., Fjaeraa, A.M., Sellegri, K., Birmili, W., Bukowiecki, N., Weingartner, E., Baltensperger, U., Zdimal, V., Zikova, N., Putaud, J.-P., Marinoni, A., Tunved, P., Hansson, H.-C., Fiebig, M., Kivekäs, N., Swietlicki, E., Lihavainen, H., Asmi, E., Ulevicius, V., Aalto, P.P., Mihalopoulos, N., Kalivitis, N., Kalapov, I., Kiss, G., de Leeuw, G., Henzing, B., O'Dowd, C., Jennings, S.G., Flentje, H., Meinhardt, F., Ries, L., Denier van der Gon, H.A.C., Visschedijk, A.J.H.

Cluster~analysis of particle number size distributions from~background sites across Europe~is presented. This generated a total of nine clusters of particle size distributions which could be further combined into two main groups, namely: a south-to-north category (four clusters) and a west-to-east category (five clusters). The first group was identified as most frequently being detected inside and around northern Germany and neighbouring countries, showing clear evidence of local afternoon nucleation and growth events that could be linked to movement of air masses from south to north arriving ultimately at the Arctic contributing to Arctic haze.~The second group of particle size spectra proved to have narrower size distributions and collectively showed a dependence of modal diameter upon the longitude of the site (west to east) at which they were most frequently detected.~These clusters indicated regional nucleation (at the coastal sites) growing to larger modes further inland. The apparent growth rate of the modal diameter was around 0.6–0.9 nm h−1. Four specific air mass back-trajectories were successively taken as case studies to examine in real time the evolution of aerosol size distributions across Europe. ~While aerosol growth processes can be observed as aerosol traverses Europe, the processes are often obscured by the addition of aerosol by emissions en route. This study revealed that some of the 24 stations exhibit more complex behaviour than others, especially when impacted by local sources or a variety of different air masses. Overall, the aerosol size distribution clustering analysis greatly simplifies the complex data set and allows a description of aerosol aging processes, which reflects the longer-term average development of particle number size distributions as air masses advect across Europe.

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.

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.

2018, Wiedensohler, A., Ma, N., Birmili, W., Heintzenberg, J., Ditas, F., Andreae, M.O., Panov, A.

Aerosol particle number size distributions (PNSD) were investigated to verify, if extremely low-volatility organic vapors (ELVOC) from natural sources alone could induce new particle formation and growth events over the remote boreal forest region of Siberia, hundreds of kilometers away from significant anthropogenic sources. We re-evaluated observations determined at a height of 300 m of the remote observatory ZOTTO (Zotino Tall Tower Observatory, http://www.zottoproject.org). We found that new particle formation events occurred only on 11 days in a 3-year period, suggesting that homogeneous nucleation with a subsequent condensational growth could not be the major process, maintaining the particle number concentration in the planetary boundary layer of the remote boreal forest area of Siberia. © 2018 Elsevier Ltd

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., Ždímal, V., Zíková, 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.

2014, Ma, N., Birmili, W., Müller, T., Tuch, T., Cheng, Y.F., Xu, W.Y., Zhao, C.S., Wiedensohler, A.

This work analyses optical properties of the dry tropospheric aerosol measured at the regional Global Atmosphere Watch (GAW) observation site Melpitz in East Germany. For a continuous observation period between 2007 and 2010, we provide representative values of the dry-state scattering coefficient, hemispheric backscattering coefficient, absorption coefficient, single scattering albedo, and scattering Ångström exponent. Besides the direct measurement, the aerosol scattering coefficient was alternatively computed from experimental particle number size distributions using a Mie model. Within pre-defined limits, a closure could be achieved with the direct measurement. The achievement of closure implies that such calculations can be used as a high-level quality control measure for data sets involving multiple instrumentation. All dry-state optical properties show pronounced annual and diurnal variations, which are attributed to the corresponding variations in the regional emission fluxes, the intensity of secondary particle formation, and the mixing layer height. Air mass classification shows that atmospheric stability is a major factor influencing the dry aerosol properties at the GAW station. In the cold season, temperature inversions limit the volume available for atmospheric mixing, so that the dry-state aerosol optical properties near the ground proved quite sensitive to the geographical origin of the air mass. In the warm season, when the atmosphere is usually well-mixed during daytime, considerably less variability was observed for the optical properties between different air masses. This work provides, on the basis of quality-checked in situ measurements, a first step towards a climatological assessment of direct aerosol radiative forcing in the region under study.

2018, Sun, J., Birmili, W., Hermann, M., Tuch, T., Weinhold, K., Spindler, G., Schladitz, A., Bastian, S., Löschau, G., Cyrys, J., Gu, J., Flentje, H., Briel, B., Asbac, C., Kaminski, H., Ries, L., Sohme, R., Gerwig, H., Wirtz, K., Meinhardt, F., Schwerin, A., Bath, O., Ma, N., Wiedensohler, A.

This work reports the first statistical analysis of multi-annual data on tropospheric aerosols from the German Ultrafine Aerosol Network (GUAN). Compared to other networks worldwide, GUAN with 17 measurement locations has the most sites equipped with particle number size distribution (PNSD) and equivalent black carbon (eBC) instruments and the most site categories in Germany ranging from city street/roadside to High Alpine. As we know, the variations of eBC and particle number concentration (PNC) are influenced by several factors such as source, transformation, transport and deposition. The dominant controlling factor for different pollutant parameters might be varied, leading to the different spatio-temporal variations among the measured parameters. Currently, a study of spatio-temporal variations of PNSD and eBC considering the influences of both site categories and spatial scale is still missing. Based on the multi-site dataset of GUAN, the goal of this study is to investigate how pollutant parameters may interfere with spatial characteristics and site categories. © 2019 The Authors