The 2017-2019 hourly particle number size distributions (PNSD) from 26 sites in Europe and 1 in the US were evaluated focusing on 16 urban background (UB) and 6 traffic (TR) sites in the framework of Research Infrastructures services reinforcing air quality monitoring capacities in European URBAN & industrial areaS (RI-URBANS) project. The main objective was to describe the phenomenology of urban ultrafine particles (UFP) in Europe with a significant air quality focus. The varying lower size detection limits made it difficult to compare PN concentrations (PNC), particularly PN_10-25, from different cities. PNCs follow a TR > UB > Suburban (SUB) order. PNC and Black Carbon (BC) progressively increase from Northern Europe to Southern Europe and from Western to Eastern Europe. At the UB sites, typical traffic rush hour PNC peaks are evident, many also showing midday-morning PNC peaks anti-correlated with BC. These peaks result from increased PN_10-25, suggesting significant PNC contributions from nucleation, fumigation and shipping. Site types to be identified by daily and seasonal PNC and BC patterns are: (i) PNC mainly driven by traffic emissions, with marked correlations with BC on different time scales; (ii) marked midday/morning PNC peaks and a seasonal anti-correlation with PNC/BC; (iii) both traffic peaks and midday peaks without marked seasonal patterns. Groups (ii) and (iii) included cities with high insolation. PNC, especially PN_25-800, was positively correlated with BC, NO₂, CO and PM for several sites. The variable correlation of PNSD with different urban pollutants demonstrates that these do not reflect the variability of UFP in urban environments. Specific monitoring of PNSD is needed if nanoparticles and their associated health impacts are to be assessed. Implementation of the CEN-ACTRIS recommendations for PNSD measurements would provide comparable measurements, and measurements of <10 nm PNC are needed for full evaluation of the health effects of this size fraction.

The MEGAPOLI (Megacities: Emissions, urban, regional and Global Atmospheric POLlution and climate effects, and Integrated tools for assessment and mitigation) experiment took place in July 2009. The aim of this campaign was to study the aging and reactions of aerosol and gas-phase emissions in the city of Paris. Three ground-based measurement sites and several mobile platforms including instrument equipped vehicles and the ATR-42 aircraft were involved. We present here the variations in particle- and gas-phase species over the city of Paris, using a combination of high-time resolution measurements aboard the ATR-42 aircraft. Particle chemical composition was measured using a compact time-of-flight aerosol mass spectrometer (C-ToF-AMS), giving detailed information on the non-refractory submicron aerosol species. The mass concentration of black carbon (BC), measured by a particle absorption soot photometer (PSAP), was used as a marker to identify the urban pollution plume boundaries. Aerosol mass concentrations and composition were affected by air-mass history, with air masses that spent longest time over land having highest fractions of organic aerosol and higher total mass concentrations. The Paris plume is mainly composed of organic aerosol (OA), BC, and nitrate aerosol, as well as high concentrations of anthropogenic gas-phase species such as toluene, benzene, and NO_x. Using BC and CO as tracers for air-mass dilution, we observe the ratio of ΔOA / ΔBC and ΔOA / ΔCO increase with increasing photochemical age (−log(NO_x / NO_y)). Plotting the equivalent ratios of different organic aerosol species (LV-OOA, SV-OOA, and HOA) illustrate that the increase in OA is a result of secondary organic aerosol (SOA) formation. Within Paris the changes in the ΔOA / ΔCO are similar to those observed during other studies in London, Mexico City, and in New England, USA. Using the measured SOA volatile organic compounds (VOCs) species together with organic aerosol formation yields, we were able to predict ~50% of the measured organics. These airborne measurements during the MEGAPOLI experiment show that urban emissions contribute to the formation of OA and have an impact on aerosol composition on a regional scale.

During the July 2011 Deriving Information on Surface conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) field experiment in Maryland, significant enhancements in Aerosol Robotic Network (AERONET) sun–sky radiometer measured aerosol optical depth (AOD) were observed in the immediate vicinity of non-precipitating cumulus clouds on some days. Both measured Ångström exponents and aerosol size distribution retrievals made before, during and after cumulus development often suggest little change in fine mode particle size; therefore, implying possible new particle formation in addition to cloud processing and humidification of existing particles. In addition to sun–sky radiometer measurements of large enhancements of fine mode AOD, lidar measurements made from both ground-based and aircraft-based instruments during the experiment also measured large increases in aerosol signal at altitudes associated with the presence of fair weather cumulus clouds. These data show modifications of the aerosol vertical profile as a result of the aerosol enhancements at and below cloud altitudes. The airborne lidar data were utilized to estimate the spatial extent of these aerosol enhancements, finding increased AOD, backscatter and extinction out to 2.5 km distance from the cloud edge. Furthermore, in situ measurements made from aircraft vertical profiles over an AERONET site during the experiment also showed large increases in aerosol scattering and aerosol volume after cloud formation as compared to before. The 15-year AERONET database of AOD measurements at the Goddard Space Flight Center (GSFC), Maryland site, was investigated in order to obtain a climatological perspective of this phenomenon of AOD enhancement. Analysis of the diurnal cycle of AOD in summer showed significant increases in AOD from morning to late afternoon, corresponding to the diurnal cycle of cumulus development.

Sea breeze (SB) phenomena may strongly influence air quality and lead to important effects on human health. In order to study the impact of SB dynamics on the properties and toxicity of aerosols, an atmospheric mobile unit was deployed during a field campaign performed in an urbanized and industrialized coastal area in Northern France. This unit combines aerosol samplers, two scanning lidars (Doppler and elastic) and an air-liquid interface (ALI, Vitrocell^®) in vitro cell exposure device. Our study highlights that after the passage of an SB front, the top of the atmospheric boundary layer collapses as the thermal internal boundary layer (TIBL) develops, which leads to high aerosol extinction coefficient values (>0.4 km⁻¹) and an increase of PM_2.5 and NO_x concentrations in the SB current. The number-size distribution of particles indicates a high proportion of fine particles (with diameter below 500 nm), while the volume-size distribution shows a major mode of coarse particles centered on 2–3 µm. Individual particle analyses performed by cryo-transmission scanning electron microscopy (cryo-TSEM)-EDX highlights that submicronic particles contained a high fraction of secondary compounds, which may result from nucleation and/or condensation of condensable species (vapors or gaseous species after photo-oxidation). Secondary aerosol (SA) formation can be enhanced in some areas, by the interaction between the SB flow and the upper continental air mass, particularly due to the effect of both turbulence and temperature/humidity gradients between these two contrasting air masses. Potential areas of SA formation are located near the ground, during the SB front passage and in the vicinity of the SB current top. During the sea breeze event, an increase in the oxidative stress and inflammation processes in exposed lung cells, compared to the unexposed cells, can also be seen. In some instances, short singularity periods are observed during SB, corresponding to a double flow structure. It consists of two adjacent SB currents that induce an important increase of the TIBL top, improving the pollutants dispersion. This is associated with a substantial decrease of aerosol mass concentrations.

During the NASA DISCOVER-AQ campaign over the US Baltimore, MD–Washington, D.C., metropolitan area in July 2011, the NASA P-3B aircraft performed extensive profiling of aerosol optical, chemical, and microphysical properties. These in situ profiles were coincident with ground-based remote sensing (AERONET) and in situ (PM_2.5) measurements. Here, we use this data set to study the correlation between the PM_2.5 observations at the surface and the column integrated measurements. Aerosol optical depth (AOD_{550 nm}) calculated with the extinction (550 nm) measured during the in situ profiles was found to be strongly correlated with the volume of aerosols present in the boundary layer (BL). Despite the strong correlation, some variability remains, and we find that the presence of aerosol layers above the BL (in the buffer layer – BuL) introduces significant uncertainties in PM_2.5 estimates based on column-integrated measurements (overestimation of PM_2.5 by a factor of 5). This suggests that the use of active remote sensing techniques would dramatically improve air quality retrievals. Indeed, the relationship between the AOD_{550 nm} and the PM_2.5 is strongly improved by accounting for the aerosol present in and above the BL (i.e., integrating the aerosol loading from the surface to the top of the BuL). Since more than 15% of the AOD values observed during DISCOVER-AQ are dominated by aerosol water uptake, the f(RH)_amb (ratio of scattering coefficient at ambient relative humidity (RH) to scattering coefficient at low RH; see Sect. 3.2) is used to study the impact of the aerosol hygroscopicity on the PM_2.5 retrievals. The results indicate that PM_2.5 can be predicted within a factor up to 2 even when the vertical variability of the f(RH)_amb is assumed to be negligible. Moreover, f(RH = 80%) and RH measurements performed at the ground may be used to estimate the f(RH)_amb during dry conditions (RH_BL < 55%).