Aerosol particles are a complex component of the atmospheric system which influence climate directly by interacting with solar radiation, and indirectly by contributing to cloud formation. The variety of their sources, as well as the multiple transformations they may undergo during their transport (including wet and dry deposition), result in significant spatial and temporal variability of their properties. Documenting this variability is essential to provide a proper representation of aerosols and cloud condensation nuclei (CCN) in climate models. Using measurements conducted in 2016 or 2017 at 62 ground-based stations around the world, this study provides the most up-to-date picture of the spatial distribution of particle number concentration (N_tot) and number size distribution (PNSD, from 39 sites). A sensitivity study was first performed to assess the impact of data availability on N_tot's annual and seasonal statistics, as well as on the analysis of its diel cycle. Thresholds of 50 % and 60 % were set at the seasonal and annual scale, respectively, for the study of the corresponding statistics, and a slightly higher coverage (75 %) was required to document the diel cycle. Although some observations are common to a majority of sites, the variety of environments characterizing these stations made it possible to highlight contrasting findings, which, among other factors, seem to be significantly related to the level of anthropogenic influence. The concentrations measured at polar sites are the lowest (∼ 10² cm⁻³) and show a clear seasonality, which is also visible in the shape of the PNSD, while diel cycles are in general less evident, due notably to the absence of a regular day–night cycle in some seasons. In contrast, the concentrations characteristic of urban environments are the highest (∼ 10³–10⁴ cm⁻³) and do not show pronounced seasonal variations, whereas diel cycles tend to be very regular over the year at these stations. The remaining sites, including mountain and non-urban continental and coastal stations, do not exhibit as obvious common behaviour as polar and urban sites and display, on average, intermediate N_tot (∼ 10²–10³ cm⁻³). Particle concentrations measured at mountain sites, however, are generally lower compared to nearby lowland sites, and tend to exhibit somewhat more pronounced seasonal variations as a likely result of the strong impact of the atmospheric boundary layer (ABL) influence in connection with the topography of the sites. ABL dynamics also likely contribute to the diel cycle of N_tot observed at these stations. Based on available PNSD measurements, CCN-sized particles (considered here as either >50 nm or >100 nm) can represent from a few percent to almost all of N_tot, corresponding to seasonal medians on the order of ∼ 10 to 1000 cm⁻³, with seasonal patterns and a hierarchy of the site types broadly similar to those observed for N_tot. Overall, this work illustrates the importance of in situ measurements, in particular for the study of aerosol physical properties, and thus strongly supports the development of a broad global network of near surface observatories to increase and homogenize the spatial coverage of the measurements, and guarantee as well data availability and quality. The results of this study also provide a valuable, freely available and easy to use support for model comparison and validation, with the ultimate goal of contributing to improvement of the representation of aerosol–cloud interactions in models, and, therefore, of the evaluation of the impact of aerosol particles on climate.

Sources and evolution of ultrafine particles were investigated both horizontally and vertically in the large urban agglomerate of Barcelona, Spain. Within the SAPUSS project (Solving Aerosol Problems by Using Synergistic Strategies), a large number of instruments was deployed simultaneously at different monitoring sites (road, two urban background, regional background, urban tower 150 m a.s.l., urban background tower site 80 m a.s.l.) during a 4 week period in September–October 2010. Particle number concentrations (N_{>5 nm}) are highly correlated with black carbon (BC) at all sites only under strong vehicular traffic influences. By contrast, under cleaner atmospheric conditions (low condensation sink, CS) such correlation diverges towards much higher N/BC ratios at all sites, indicating additional sources of particles including secondary production of freshly nucleated particles. Size-resolved aerosol distributions (N_10–500) as well as particle number concentrations (N_{>5 nm}) allow us to identify three types of nucleation and growth events: (1) a regional type event originating in the whole study region and impacting almost simultaneously the urban city of Barcelona and the surrounding urban background area; (2) a regional type event impacting only the regional background area but not the urban agglomerate; (3) an urban type event which originates only within the city centre but whose growth continues while transported away from the city to the regional background. Furthermore, during these clean air days, higher N are found at tower level than at ground level only in the city centre whereas such a difference is not so pronounced at the remote urban background tower. In other words, this study suggests that the column of air above the city ground level possesses the optimal combination between low CS and high vapour source, hence enhancing the concentrations of freshly nucleated particles. By contrast, within stagnant polluted atmospheric conditions, higher N and BC concentrations are always measured at ground level relative to tower level at all sites. Our study suggests that the city centre of Barcelona is a source of non-volatile traffic primary particles (29–39% of N_{>5 nm}), but other sources, including secondary freshly nucleated particles contribute up to 61–71% of particle number (N_{>5 nm}) at all sites. We suggest that organic compounds evaporating from freshly emitted traffic particles are a possible candidate for new particle formation within the city and urban plume.

The vertical profile of new particle formation (NPF) events was studied by comparing the aerosol size number distributions measured aloft and at surface level in a suburban environment in Madrid, Spain, using airborne instruments. The horizontal distribution and regional impact of the NPF events was investigated with data from three urban, urban background, and suburban stations in the Madrid metropolitan area. Intensive regional NPF episodes followed by particle growth were simultaneously recorded at three stations in and around Madrid during a field campaign in July 2016. The urban stations presented larger formation rates compared to the suburban station. Condensation and coagulation sinks followed a similar evolution at all stations, with higher values at urban stations. However, the total number concentration of particles larger than 2.5 nm was lower at the urban station and peaked around noon, when black carbon (BC) levels are at a minimum. The vertical soundings demonstrated that ultrafine particles (UFPs) are formed exclusively inside the mixed layer. As convection becomes more effective and the mixed layer grows, UFPs are detected at higher levels. The morning soundings revealed the presence of a residual layer in the upper levels in which aged particles (nucleated and grown on previous days) prevail. The particles in this layer also grow in size, with growth rates significantly smaller than those inside the mixed layer. Under conditions with strong enough convection, the soundings revealed homogeneous number size distributions and growth rates at all altitudes, which follow the same evolution at the other stations considered in this study. This indicates that UFPs are detected quasi-homogenously in an area spanning at least 17 km horizontally. The NPF events extend over the full vertical extension of the mixed layer, which can reach as high as 3000 m in the area, according to previous studies. On some days a marked decline in particle size (shrinkage) was observed in the afternoon, associated with a change in air masses. Additionally, a few nocturnal nucleation-mode bursts were observed at the urban stations, for which further research is needed to elucidate their origin.

Red Española de DMAs Ambientales (REDMAAS), the Spanish network of environmental differential mobility analyzers (DMAs), currently comprises six research groups involved in the measurement of atmospheric aerosol size distributions by means of DMAs. The aim of this network is to guarantee the good quality and comparability of the routine measurements carried out at each location and in diverse environments across Spain. In order to achieve this objective, one of its main activities is the annual intercomparison of mobility size spectrometers used within the network (five units of scanning mobility particle sizers [SMPS] and one ultrafine particle monitor [UFPM]). Here we report the 2main results obtained during the 2010–2012 campaigns, including a study on particle deposition in dryers used in ambient air sampling systems. In general, all instruments showed good performance with deviations in accepted tolerance. The intercomparisons have been proved to be a useful exercise to detect instrument problems, such as incorrect calibrations. DMA calibration checks were performed with polystyrene latex reference particles. Deviations of less than 1% were observed during the first year, which increased 4.7% during the last campaign. Some differences among the responses of different condensation particle counter (CPC) models were encountered, being mainly connected to the intrinsic characteristics of each counter. The comparison of UFPM with CPCs has given good results. The SMPS intercomparisons, especially for particles above 20 nm, have been within +/−15% tolerance. Regarding particle deposition in dryers used in sampling systems, particle penetration was lower than predicted by the recommended model. This result was probably due to the fact that not all the possible mechanisms were considered in the model. Copyright 2015 American Association for Aerosol Research