Primary Versus Secondary Contributions to Particle Number Concentrations in the European Boundary Layer

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.JRC.H.2-Air and Climat

Tropospheric and stratospheric smoke over Europe as observed within EARLINET/ACTRIS in summer 2017

For several weeks in summer 2017, strong smoke layers were observed over Europe at numerous EARLINET stations. EARLINET is the European research lidar network and part of ACTRIS and comprises more than 30 ground-based lidars. The smoke layers were observed in the troposphere as well as in the stratosphere up to 25 km from Northern Scandinavia over whole western and central Europe to the Mediterranean regions. Backward trajectory analysis among other tools revealed that these smoke layers originated from strong wild fires in western Canada in combination with pyrocumulus convection. An extraordinary fire event in the mid of August caused intense smoke layers that were observed across Europe for several weeks starting on 18 August 2017. Maximum aerosol optical depths up to 1.0 at 532 nm were observed at Leipzig, Germany, on 22 August 2017 during the peak of this event. The stratospheric smoke layers reached extinction coefficient values of more than 600 Mm−1 at 532 nm, a factor of 10 higher than observed for volcanic ash after the Pinatubo eruption in the 1990s. First analyses of the intensive optical properties revealed low particle depolarization values at 532 nm for the tropospheric smoke (spherical particles) and rather high values (up to 20%) in the stratosphere. However, a strong wavelength dependence of the depolarization ratio was measured for the stratospheric smoke. This indicates irregularly shaped stratospheric smoke particles in the size range of the accumulation mode. This unique depolarization feature makes it possible to distinguish clearly smoke aerosol from cirrus clouds or other aerosol types by polarization lidar measurements. Particle extinction-to-backscatter ratios were rather low in the order of 40 to 50 sr at 355 nm, while values between 70-90 sr were measured at higher wavelengths. In the western and central Mediterranean, stratospheric smoke layers were most prominent in the end of August at heights between 16 and 20 km. In contrast, stratospheric smoke started to occur in the eastern Mediterranean (Cyprus and Israel) in the beginning of September between 18 and 23 km. Stratospheric smoke was still visible in the beginning of October at certain locations (e.g. Evora, Portugal), while tropospheric smoke was mainly observed until the end of August within Europe. An overview of the smoke layers measured at several EARLINET sites will be given. The temporal development of these layers as well as their geometrical and optical properties will be presented

Seasonality of the particle number concentration and size distribution : a global analysis retrieved from the network of Global Atmosphere Watch (GAW) near-surface observatories

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 (similar to 10(2) 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 (similar to 10(3)-10(4) 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 (similar to 10(2)-10(3) 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 similar to 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.Peer reviewe

Precipitation scavenging of aerosol particles at a rural site in the Czech Republic

The influence of in-cloud and below-cloud scavenging, described by the obscurities (mist, fog and shallow fog) and precipitation, on submicron atmospheric aerosol (AA) particle number size distributions (PNSDs) was studied using 5 years of measurements at the rural background station Kosˇetice. The typical PNSDs during individual meteorological phenomena were compared, and the change in the concentrations before and after the beginning of the phenomenon, the scavenging coefficient ls, and the rate of change of the AA concentrations with time were computed. It was found that both obscurities and precipitation have a strong influence on theAAconcentrations, both on the total number concentrations and on the PNSDs. The presence of phenomena even changes the number of modes on the PNSDs. The PNSD main mode is shifted to the larger particles, and the concentrations of particles smaller than 50 nm in diameter are considerably lower. In nucleation mode, however, wet scavenging does not seem to be the main process influencing the AA concentrations, although its considerable effect on the concentration was proved. During obscurities, there is a typical PNSD to which the PNSDs converge at any mist/fog/shallow fog event. The concentrations of AA particles smaller than 80 nm are lower than they are during periods without any phenomenon recorded, and the concentrations of the strongly prevailing accumulation mode are higher. During liquid precipitation, PNSDs are lower when compared to non-event periods. With larger droplets of the phenomenon, the position of the main mode of the bimodal PNSDs is shifted to the smaller particles. The process of gas-to-particle conversion takes place in the breaks from precipitation during a rain showers period. Precipitation containing frozen hydrometeors behaves differently from liquid precipitation. Concentrations of AA particles larger than 200 nm during precipitation containing solid particles do not differ from non-event cases, suggesting insignificant scavenging

Modal Structure of the Fine Urban Aerosol in four European Cities

The size distribution of the sub micrometer aerosol number concentration in the urban Environment appears to display a statistically significant modal structure (Van Dingenen et al., 2004). This depends on a number of factors such as local atmospheric conditions, density and type of emissions. The development of certain "universal" aerosol number distribution patterns can contribute towards the assessment of human exposure to fine particulate matter or facilitate the characterization of certain emission sources and their impact on air quality. Here, preliminary results from the analysis of measured number size distributions are presented for four European cities.JRC.H.4-Transport and air qualit

Manikin-based size-resolved penetrations of CE-marked filtering facepiece respirators

Summarization: The purpose of this manikin-based study was to determine the percentage penetrations of nine CE-marked filtering facepiece respirator models (two samples from each) from filtering classes FFP1, FFP2, and FFP3 and to demonstrate by an independent measurement method the disadvantages and shortcomings of the currently valid European Norm (EN 149: 2001) for filtering facepieces. All of the filtering facepieces were evaluated size-selectively in an experimental chamber using charge-neutralized monodisperse ammonium sulfate in 9 sizes ranging from 20-400 nm of count median diameter (CMD) under flowrate of 95 L/min. The results were then compared to the previous study concerning penetrations of 47-mm diameter filters cut from the filtering material of identical filtering facepieces. Although these two experimental methods for measuring penetrations of filtering materials from filtering facepieces are in good agreement (R-2 = 0.91), the results show within-respirator variations in all three filtering classes (5.5-19.3% for all FFRs in FFP1, 2.8-8.5% in FFP2, and 0.1-2.8% in FFP3). The most penetrating particle size (MPPS) in this study was found to be in the range of 25-65 nm (CMD), which is in agreement with the range of 30-60 nm found in the previous study. Moreover, 7 out of 9 FFR models reached higher penetrations from manikin-based respirator measurements than during measurements of filters from the respective respirators. Furthermore, penetration levels increased up to similar to 50% when the respirator was not sealed around the face of the manikin, indicating that the real protection level provided by these filtering facepieces may be even lower if the respirator does not fit perfectly. Considering that poor filtration efficiency and poor fit may increase under real work conditions, the particle penetration is even higher than was found in this study. Therefore, the CE-marked respirators examined in this study may not be efficient in providing the expected level of protection for workers exposed to nanoparticlesPresented on: Journal of Occupational and Environmental Hygien

Markers of Oxidative Stress in the Exhaled Breath Condensate of Workers Handling Nanocomposites

Researchers in nanocomposite processing may inhale a variety of chemical agents, including nanoparticles. This study investigated airway oxidative stress status in the exhaled breath condensate (EBC). Nineteen employees (42.4 ± 11.4 y/o), working in nanocomposites research for 18.0 ± 10.3 years were examined pre-shift and post-shift on a random workday, together with nineteen controls (45.5 ± 11.7 y/o). Panels of oxidative stress biomarkers derived from lipids, nucleic acids, and proteins were analyzed in the EBC. Aerosol exposures were monitored during three major nanoparticle generation operations: smelting and welding (workshop 1) and nanocomposite machining (workshop 2) using a suite of real-time and integrated instruments. Mass concentrations during these operations were 0.120, 1.840, and 0.804 mg/m3, respectively. Median particle number concentrations were 4.8 × 104, 1.3 × 105, and 5.4 × 105 particles/cm3, respectively. Nanoparticles accounted for 95, 40, and 61%, respectively, with prevailing Fe and Mn. All markers of nucleic acid and protein oxidation, malondialdehyde, and aldehydes C6–C13 were elevated, already in the pre-shift samples relative to controls in both workshops. Significant post-shift elevations were documented in lipid oxidation markers. Significant associations were found between working in nanocomposite synthesis and EBC biomarkers. More research is needed to understand the contribution of nanoparticles from nanocomposite processing in inducing oxidative stress, relative to other co-exposures generated during welding, smelting, and secondary oxidation processes, in these workshops

Deep Airway Inflammation and Respiratory Disorders in Nanocomposite Workers

Thousands of researchers and workers worldwide are employed in nanocomposites manufacturing, yet little is known about their respiratory health. Aerosol exposures were characterized using real time and integrated instruments. Aerosol mass concentration ranged from 0.120 mg/m3 to 1.840 mg/m3 during nanocomposite machining processes; median particle number concentration ranged from 4.8 × 104 to 5.4 × 105 particles/cm3. The proportion of nanoparticles varied by process from 40 to 95%. Twenty employees, working in nanocomposite materials research were examined pre-shift and post-shift using spirometry and fractional exhaled nitric oxide (FeNO) in parallel with 21 controls. Pro-inflammatory leukotrienes (LT) type B4, C4, D4, and E4; tumor necrosis factor (TNF); interleukins; and anti-inflammatory lipoxins (LXA4 and LXB4) were analyzed in their exhaled breath condensate (EBC). Chronic bronchitis was present in 20% of researchers, but not in controls. A significant decrease in forced expiratory volume in 1 s (FEV1) and FEV1/forced vital capacity (FVC) was found in researchers post-shift (p ˂ 0.05). Post-shift EBC samples were higher for TNF (p ˂ 0.001), LTB4 (p ˂ 0.001), and LTE4 (p ˂ 0.01) compared with controls. Nanocomposites production was associated with LTB4 (p ˂ 0.001), LTE4 (p ˂ 0.05), and TNF (p ˂ 0.001), in addition to pre-shift LTD4 and LXB4 (both p ˂ 0.05). Spirometry documented minor, but significant, post-shift lung impairment. TNF and LTB4 were the most robust markers of biological effects. Proper ventilation and respiratory protection are required during nanocomposites processing