Search

Black carbon (BC) is a major component of submicron particulate matter (PM), with significant health and climate impacts. Many cities in emerging countries lack comprehensive knowledge about BC emissions and exposure levels. This study investigates BC concentration levels, identifies its emission sources, and characterizes the optical properties of BC at urban background sites of the two largest high-altitude Bolivian cities: La Paz (LP) (3600 m above sea level) and El Alto (EA) (4050 m a.s.l.), where atmospheric oxygen levels and intense radiation may affect BC production. The study relies on concurrent measurements of equivalent black carbon (eBC), elemental carbon (EC), and refractory black carbon (rBC) and their comparison with analogous data collected at the nearby Chacaltaya Global Atmosphere Watch Station (5240 m a.s.l). The performance of two independent source apportionment techniques was compared: a bilinear model and a least-squares multilinear regression (MLR). Maximum eBC concentrations were observed during the local dry season (LP: eBC = 1.5 ± 1.6 µg m−3; EA: 1.9±2.0 µg m−3). While eBC concentrations are lower at the mountain station, daily transport from urban areas is evident. Average mass absorption cross sections of 6.6–8.2 m2 g−1 were found in the urban area at 637 nm. Both source apportionment methods exhibited a reasonable level of agreement in the contribution of biomass burning (BB) to absorption. The MLR method allowed the estimation of the contribution and the source-specific optical properties for multiple sources, including open waste burning.

As an important source of sub-micrometer particles, atmospheric new particle formation (NPF) has been observed in various environments. However, most studies provide little more than snapshots of the NPF process due to their underlying observations being limited in space and time. To obtain statistically relevant evidence on NPF across various environments, we investigated the characteristics of NPF based on a 5-year dataset of the German Ultrafine Aerosol Network (GUAN). The results were also compared with observations in previous studies, with the aim to depict a relatively complete picture of NPF in central Europe. The highest NPF occurrence frequency was observed in regional background sites, with an average of about 19 %, followed by urban background (15 %), low-mountain-range (7 %), and high Alpine (3 %) sites. The annual mean growth rate between 10 and 25 nm varied from 3.7–4.7 nm h−1, while the formation rate with same size range 10–25 nm from 0.4 to 2.9 cm−3 s−1. The contribution of NPF to ultrafine particles (UFPs) was about 13 %, 21 %, and 7 % for the urban background, regional background, and low mountain range, respectively. The influence of NPF on cloud condensation nuclei (CCN) number concentration and the aerosol extinction coefficient for NPF days was the highest in mountainous areas. These findings underscore the importance of local environments when assessing the potential impact of NPF on regional climate in models, and they also emphasize the usefulness of a long-term aerosol measurement network for understanding the variation in NPF features and their influencing factors over a regional scale.

The oceanic emission of dimethyl sulfide (DMS) plays a vital role in the Earth's climate system and constitutes a substantial source of uncertainty when evaluating aerosol radiative forcing. Currently, the widely used monthly climatology of sea surface DMS concentration falls short of meeting the requirement for accurately simulating DMS-derived aerosols with chemical transport models. Hence, there is an urgent need for a high-resolution, multi-year global sea surface DMS dataset. Here we develop an artificial neural network ensemble model that uses nine environmental factors as input features and captures the variability of the DMS concentration across different oceanic regions well. Subsequently, a global sea surface DMS concentration and flux dataset (1° × 1°) with daily resolution spanning from 1998 to 2017 is established. According to this dataset, the global annual average concentration was ∼ 1.71 nM, and the annual total emissions were ∼ 17.2 Tg S yr−1, with ∼ 60 % originating from the Southern Hemisphere. While overall seasonal variations are consistent with previous DMS climatologies, notable differences exist in regional-scale spatial distributions. The new dataset enables further investigations into daily and decadal variations. Throughout the period 1998–2017, the global annual average concentration exhibited a slight decrease, while total emissions showed no significant trend. The DMS flux from our dataset showed a stronger correlation with the observed atmospheric methanesulfonic acid concentration compared to those from previous monthly climatologies. Therefore, it can serve as an improved emission inventory of oceanic DMS and has the potential to enhance the simulation of DMS-derived aerosols and associated radiative effects. The new DMS gridded products are available at https://doi.org/10.5281/zenodo.11879900 (Zhou et al., 2024).

There is a body of evidence that ultrafine particles (UFP, those with diameters ≤ 100 nm) might have significant impacts on health. Accordingly, identifying sources of UFP is essential to develop abatement policies. This study focuses on urban Europe, and aims at identifying sources and quantifying their contributions to particle number size distribution (PNSD) using receptor modelling (Positive Matrix Factorization, PMF), and evaluating long-term trends of these source contributions using the non-parametric Theil-Sen’s method. Datasets evaluated include 14 urban background (UB), 5 traffic (TR), 4 suburban background (SUB), and 1 regional background (RB) sites, covering 18 European and 1 USA cities, over the period, when available, from 2009 to 2019. Ten factors were identified (4 road traffic factors, photonucleation, urban background, domestic heating, 2 regional factors and long-distance transport), with road traffic being the primary contributor at all UB and TR sites (56–95 %), and photonucleation being also significant in many cities. The trends analyses showed a notable decrease in traffic-related UFP ambient concentrations, with statistically significant decreasing trends for the total traffic-related factors of −5.40 and −2.15 % yr−1 for the TR and UB sites, respectively. This abatement is most probably due to the implementation of European emissions standards, particularly after the introduction of diesel particle filters (DPFs) in 2011. However, DPFs do not retain nucleated particles generated during the dilution of diesel exhaust semi-volatile organic compounds (SVOCs). Trends in photonucleation were more diverse, influenced by a reduction in the condensation sink potential facilitating new particle formation (NPF) or by a decrease in the emissions of UFP precursors. The decrease of primary PM emissions and precursors of UFP also contributed to the reduction of urban and regional background sources.

Studies revealed airports as a prominent source of ultrafine particles (UFP), which can disperse downwind to residential areas, raising health concerns. To expand our understanding of how air traffic-related emissions influence total particle number concentration (PNC) in the airport’s surrounding areas, we conduct long-term assessment of airborne particulate exposure before and after relocation of air traffic from “Otto Lilienthal” Airport (TXL) to Berlin Brandenburg Airport “Willy Brandt” (BER) in Berlin, Germany. Here, we provide insights into the spatial–temporal variability of PNC measured in 16 schools recruited for Berlin-Brandenburg Air Study (BEAR).The results show that the average PNC in Berlin was 7900 ± 7000 cm−3, consistent with other European cities. The highest median PNC was recorded in spring (6700 cm−3) and the lowest in winter (5100 cm−3). PNC showed a bi-modal increase during morning and evening hours at most measurement sites due to road-traffic emissions. A comparison between measurements at the schools and fixed monitoring sites revealed good agreement at distances up to 5 km. A noticeable decline in this agreement occurred as the distance between measurement sites increased. After TXL was closed, PNC in surrounding areas decreased by 30 %. The opposite trend was not seen after BER was re-opened after the COVID-lock-down, as the air traffic has not reached the full capacity yet. The analysis of particle number size distribution data showed that UFP number fraction exhibit seasonal variations, with higher values in spring and autumn. This can be explained by nucleation events, which notably affected PNC.The presented findings will play a pivotal role in forthcoming source attribution and epidemiological investigations, offering a holistic understanding of airports’ impact on airborne pollutant levels and their health implications. The study calls for further investigations of air-traffic-related physical–chemical pollutant properties in areas found further away (> 10 km) from airports.

Abstract In recent years, researchers have emphasized the use of fractal aggregate morphology instead of the core-shell morphology in global climate models for estimating black carbon (BC) forcing. This study confirms that fractal morphology plays an important role in reducing the overestimation of aerosol light absorption calculations in the case of an urban polluted environment. During periods of high anthropogenic BC emissions at Delhi, the particle light absorption is overestimated by 50 to 200% by assumptions of both external mixing and internal core-shell mixing. While incorporating the aggregate morphology model into light absorption simulations is beneficial in such cases, it comes with a high computational burden. To address this, we propose a metric known as morphology index (MI). This index distributes the weightage between the two extreme cases of core-shell and fractal aggregate to obtain accurate particle light absorption. Long-range transported aerosols were estimated to have an MI of 0.78, and fresh local emissions had an MI of 0.48. A BC-based aerosol classification approach was developed to determine the most relevant particle size mode for light absorption. The method is based on patterns found between the correlations of the BC mass concentrations and aerosol number concentrations at the different particles sizes (BC-size correlation spectra). BC-size correlation spectra are introduced as a concept that may be used (i) independently to understand the size-dependent heterogeneous distribution of aerosol light absorption and (ii) in conjunction with MI to accurately model the optical properties of aerosols in different BC regimes.

Recent research has revealed the crucial role of wintertime, episodic high chloride (H-Cl) emissions in the Delhi region, which significantly impact aerosol hygroscopicity and aerosol-bound liquid water, thus contributing to the initiation of Delhi fog episodes. However, these findings have primarily relied on modeled aerosol hygroscopicity, necessitating validation through direct hygroscopicity measurements. This study presents the measurements of non-refractory bulk aerosol composition of PM1 from an Aerodyne aerosol chemical speciation monitor and for first-time size-resolved hygroscopic growth factors (nucleation, Aitken, and accumulated mode particles) along with their associated hygroscopicity parameters at 90 % relative humidity using a hygroscopic tandem differential mobility analyzer at the Delhi Aerosol Supersite. Our observations demonstrate that the hygroscopicity parameter for aerosol particles varies from 0.00 to 0.11 (with an average of 0.03 ± 0.02) for 20 nm particles, 0.05 to 0.22 (0.11 ± 0.03) for 50 nm particles, 0.05 to 0.30 (0.14 ± 0.04) for 100 nm particles, 0.05 to 0.41 (0.18 ± 0.06) for 150 nm particles, and 0.05 to 0.56 (0.22 ± 0.07) for 200 nm particles. Surprisingly, our findings demonstrate that the period with H-Cl emissions displays notably greater hygroscopicity (0.35 ± 0.06) in comparison to spans marked by high biomass burning (0.18 ± 0.04) and high hydrocarbon-like organic aerosol (0.17 ± 0.05) and relatively cleaner periods (0.27 ± 0.07). This research presents initial observational proof that ammonium chloride is the main factor behind aerosol hygroscopic growth and aerosol-bound liquid water content in Delhi. The finding emphasizes ammonium chloride's role in aerosol–water interaction and related haze/fog development. Moreover, the high chloride levels in aerosols seem to prevent the adverse impact of high organic aerosol concentrations on cloud condensation nuclei activity.

The chemical composition of PM10 and non-overlapping PM2.5 was studied at the summit of Mt. Chacaltaya (5380 m a.s.l., lat. −16.346950°, long. −68.128250°) providing a unique long-term record spanning from December 2011 to March 2020. The chemical composition of aerosol at the Chacaltaya Global Atmosphere Watch (GAW) site is representative of the regional background, seasonally affected by biomass burning practices and by nearby anthropogenic emissions from the metropolitan area of La Paz–El Alto. Concentration levels are clearly influenced by seasons with minima occurring during the wet season (December to March) and maxima occurring during the dry and transition seasons (April to November). Ions, total carbon (EC + OC), and saccharide interquartile ranges for concentrations are 558–1785, 384–1120, and 4.3–25.5 ng m−3 for bulk PM10 and 917–2308, 519–1175, and 3.9–24.1 ng m−3 for PM2.5, respectively, with most of the aerosol seemingly present in the PM2.5 fraction. Such concentrations are overall lower compared to other high-altitude stations around the globe but higher than Amazonian remote sites (except for OC). For PM10, there is dominance of insoluble mineral matter (33 %–56 % of the mass), organic matter (7 %–34 %), and secondary inorganic aerosol (15 %–26 %). Chemical composition profiles were identified for different origins: EC, NO3-, NH4+, glucose, and C2O42- for the nearby urban and rural areas; OC, EC, NO3-, K+, acetate, formate, levoglucosan, and some F− and Br− for biomass burning; MeSO3-, Na+, Mg2+, K+, and Ca2+ for aged marine emissions from the Pacific Ocean; arabitol, mannitol, and glucose for biogenic emissions; Na+, Ca2+, Mg2+, and K+ for soil dust; and SO42-, F−, and some Cl− for volcanism. Regional biomass burning practices influence the soluble fraction of the aerosol between June and November. The organic fraction is present all year round and has both anthropogenic (biomass burning and other combustion sources) and natural (primary and secondary biogenic emissions) origins, with the OC/EC mass ratio being practically constant all year round (10.5 ± 5.7, IQR 8.1–13.3). Peruvian volcanism has dominated the SO42- concentration since 2014, though it presents strong temporal variability due to the intermittence of the sources and seasonal changes in the transport patterns. These measurements represent some of the first long-term observations of aerosol chemical composition at a continental high-altitude site in the tropical Southern Hemisphere.

Recent years have seen an increase in the use of wood for energy production of over 30 %, and this trend is expected to continue due to the current energy crisis and geopolitical instability. At present, residential wood burning (RWB) is one of the most important sources of organic aerosols (OAs) and black carbon (BC), posing a significant risk to air quality and health. Simultaneously, as a substantial aerosol source, RWB also holds relevance in the context of aerosol radiative effects and climate. While BC is recognized for its large light absorption cross-section, the role of OAs in light absorption is still under evaluation due to their heterogeneous composition and source-dependent optical properties. Existing studies that characterize wood-burning aerosol emissions in Europe primarily concentrate on urban and background sites and focus on BC properties. Despite the significant RWB emissions in rural areas, these locations have received comparatively less attention. The present scenario underscores the imperative for an improved understanding of RWB pollution, aerosol optical properties, and their subsequent connection to climate impacts, particularly in rural areas. We have characterized atmospheric aerosol particles from a central European rural site during wintertime in the village of Retje in Loški Potok, Slovenia, from 1 December 2017 to 7 March 2018. The village experienced extremely high aerosol concentrations produced by RWB and near-ground temperature inversion. The isolated location of the site and the substantial local emissions made it an ideal laboratory-like place for characterizing RWB aerosols with low influence from non-RWB sources under ambient conditions. The mean mass concentrations of OA and BC were 35 µg m−3 (max⁡=270 µg m−3) and 3.1 µg m−3 (max⁡=24 µg m−3), respectively. The mean total particle number concentration (10–600 nm) was 9.9×103 particles cm−3 (max⁡=59×103 particles cm−3). The mean total light absorption coefficients at 370 and 880 nm measured by an AE33 Aethalometer were 120 and 22 Mm−1 and had maximum values of 1100 and 180 Mm−1, respectively. The aerosol concentrations and absorption coefficients measured during the campaign in Loški Potok were significantly larger than reported values for several urban areas in the region with larger populations and a larger extent of aerosol sources. Here, considerable contributions from brown carbon (BrC) to the total light absorption were identified, reaching up to 60 % and 48 % in the near-UV (370 nm) and blue (470 nm) wavelengths. These contributions are up to 3 times higher than values reported for other sites impacted by wood-burning emissions. The calculated mass absorption cross-section and the absorption Ångström exponent for RWB OA were MACOA,370nm=2.4 m2 g−1, and AAEBrC,370-590nm=3.9, respectively. Simple-forcing-efficiency (SFE) calculations were performed as a sensitivity analysis to evaluate the climate impact of the RWB aerosols produced at the study site by integrating the optical properties measured during the campaign. The SFE results show a considerable forcing capacity from the local RWB aerosols, with a high sensitivity to OA absorption properties and a more substantial impact over bright surfaces like snow, typical during the coldest season with higher OA emissions from RWB. Our study's results are highly significant regarding air pollution, optical properties, and climate impact. The findings suggest that there may be an underestimation of RWB emissions in rural Europe and that further investigation is necessary.

Early growth of atmospheric particles is essential for their survival and ability to participate in cloud formation. Many different atmospheric vapors contribute to the growth, but even the main contributors still remain poorly identified in many environments, such as high-altitude sites. Based on measured organic vapor and sulfuric acid concentrations under ambient conditions, particle growth during new particle formation events was simulated and compared with the measured particle size distribution at the Chacaltaya Global Atmosphere Watch station in Bolivia (5240 m a.s.l.) during April and May 2018, as a part of the SALTENA (Southern Hemisphere high-ALTitude Experiment on particle Nucleation and growth) campaign. Despite the challenging topography and ambient conditions around the station, the simple particle growth model used in the study was able to show that the detected vapors were sufficient to explain the observed particle growth, although some discrepancies were found between modeled and measured particle growth rates. This study, one of the first of such studies conducted on high altitude, gives insight on the key factors affecting the particle growth on the site and helps to improve the understanding of important factors on high-altitude sites and the atmosphere in general. Low-volatility organic compounds originating from multiple surrounding sources such as the Amazonia and La Paz metropolitan area were found to be the main contributor to the particle growth, covering on average 65 % of the simulated particle mass in particles with a diameter of 30 nm. In addition, sulfuric acid made a major contribution to the particle growth, covering at maximum 37 % of the simulated particle mass in 30 nm particles during periods when volcanic activity was detected on the area, compared to around 1 % contribution on days without volcanic activity. This suggests that volcanic emissions can greatly enhance the particle growth.

A profound knowledge of pollutant emissions and transport processes is essential to better assess the impact on local air quality, which ultimately affects human health. This is of special importance in the proximity of airports, as flight activities are a major source of ultrafine aerosol particles (UFP) that are associated with adverse health effects. A quantification of the aerosol population in the horizontal and in particular in the vertical distribution has not been sufficiently characterized so far, but is of crucial relevance, as the atmospheric boundary layer (ABL) is strongly interacting with aerosols. For this purpose, the fixed-wing research drone called ALADINA (Application of Light-weight Aircraft for Detecting in-situ Aerosol) was operated at a distance of approximately 4 km downwind of the German airport Berlin Brandenburg (BER) on October 11–19, 2021. During the investigation period, 140 vertical profiles of different meteorological parameters and aerosol particle sizes were obtained on six measurement days between the surface and up to a maximum altitude of 750 m above ground level (a.g.l.). The investigations indicate several features: The stability of the ABL is a key characteristic for the vertical distribution of aerosol population with highest concentrations close to ground. Inversion layers further enhance horizontal transport so that airport pollutants can be moved to a further distance away. The airborne observations of total particle number concentration (TNC) coincide with ground-based data from fix-point sites. They show a high variability depending on the distance to the plume as well as upwind position and highest concentrations of TNC related to rush hours of airport operations.

The European Metrology Research Programme participating countries and the European Union jointly fund a three year project to address the need of the automotive industry for a metrological sound base for exhaust measurements. The collaborative work on particle emissions involves five European National Metrology Institutes, the Tampere University of Technology, the Joint Research Centre for Energy and Transport and the Leibniz Institute for Tropospheric Research. On one hand, a particle number and size standard for soot particles is aimed for. Eventually this will allow the partners to provide accurate and comparable calibrations of measurement instruments for the type approval of Euro 5b and Euro 6 vehicles. Calibration aerosols of combustion particles, silver and graphite proof partially suitable. Yet, a consensus choice together with instrument manufactures is pending as the aerosol choice considerably affects the number concentration measurement. Furthermore, the consortium issued consistent requirements for novel measuring instruments foreseen to replace today’s opacimeters in regulatory periodic emission controls of soot and compared them with European legislative requirements. Four partners are conducting a metrological validation of prototype measurement instruments. The novel instruments base on light scattering, electrical, ionisation chamber and diffusion charging sensors and will be tested at low and high particle concentrations. Results shall allow manufacturers to further improve their instruments to comply with legal requirements.

La Paz and El Alto are two fast-growing, high-altitude Bolivian cities forming the second-largest metropolitan area in the country. Located between 3200 and 4050 m a.s.l. (above sea level), these cities are home to a burgeoning population of approximately 1.8 million residents. The air quality in this conurbation is heavily influenced by urbanization; however, there are no comprehensive studies evaluating the sources of air pollution and their health impacts. Despite their proximity, the substantial variation in altitude, topography, and socioeconomic activities between La Paz and El Alto result in distinct sources, dynamics, and transport of particulate matter (PM). In this investigation, PM10 samples were collected at two urban background stations located in La Paz and El Alto between April 2016 and June 2017. The samples were later analyzed for a wide range of chemical species including numerous source tracers (OC, EC, water-soluble ions, sugar anhydrides, sugar alcohols, trace metals, and molecular organic species). The United States Environmental Protection Agency (U.S. EPA) Positive Matrix Factorization (PMF v.5.0) receptor model was employed for the source apportionment of PM10. This is one of the first source apportionment studies in South America that incorporates an extensive suite of organic markers, including levoglucosan, polycyclic aromatic hydrocarbons (PAHs), hopanes, and alkanes, alongside inorganic species. The multisite PMF resolved 11 main sources of PM. The largest annual contribution to PM10 came from the following two major sources: the ensemble of the four vehicular emissions sources (exhaust and non-exhaust), accountable for 35 % and 25 % of the measured PM in La Paz and El Alto, respectively; and dust, which contributed 20 % and 32 % to the total PM mass. Secondary aerosols accounted for 22 % (24 %) in La Paz (El Alto). Agricultural smoke resulting from biomass burning in the Bolivian lowlands and neighboring countries contributed to 9 % (8 %) of the total PM10 mass annually, increasing to 17 % (13 %) between August–October. Primary biogenic emissions were responsible for 13 % (7 %) of the measured PM10 mass. Additionally, a profile associated with open waste burning occurring from May to August was identified. Although this source contributed only to 2 % (5 %) of the total PM10 mass, it constitutes the second largest source of PAHs, which are compounds potentially hazardous to human health. Our analysis additionally resolved two different traffic-related factors, a lubricant source (not frequently identified), and a non-exhaust emissions source. Overall, this study demonstrates that PM10 concentrations in La Paz and El Alto region are predominantly influenced by a limited number of local sources. In conclusion, to improve air quality in both cities, efforts should primarily focus on addressing dust, traffic emissions, open waste burning, and biomass burning.

To fight against the first wave of coronavirus disease 2019 (COVID-19) in 2020, lockdown measures were implemented in most European countries. These lockdowns had well-documented effects on human mobility. We assessed the impact of the lockdown implementation and relaxation on air pollution by comparing daily particulate matter (PM), nitrogen dioxide (NO2) and ozone (O3) concentrations, as well as particle number size distributions (PNSDs) and particle light absorption coefficient in situ measurement data, with values that would have been expected if no COVID-19 epidemic had occurred at 28 sites across Europe for the period 17 February–31 May 2020. Expected PM, NO2 and O3 concentrations were calculated from the 2020 Copernicus Atmosphere Monitoring Service (CAMS) ensemble forecasts, combined with 2019 CAMS ensemble forecasts and measurement data. On average, lockdown implementations did not lead to a decrease in PM2.5 mass concentrations at urban sites, while relaxations resulted in a +26 ± 21 % rebound. The impacts of lockdown implementation and relaxation on NO2 concentrations were more consistent (−29 ± 17 and +31 ± 30 %, respectively). The implementation of the lockdown measures also induced statistically significant increases in O3 concentrations at half of all sites (+13 % on average). An enhanced oxidising capacity of the atmosphere could have boosted the production of secondary aerosol at those places. By comparison with 2017–2019 measurement data, a significant change in the relative contributions of wood and fossil fuel burning to the concentration of black carbon during the lockdown was detected at 7 out of 14 sites. The contribution of particles smaller than 70 nm to the total number of particles significantly also changed at most of the urban sites, with a mean decrease of −7 ± 5 % coinciding with the lockdown implementation. Our study shows that the response of PM2.5 and PM10 mass concentrations to lockdown measures was not systematic at various sites across Europe for multiple reasons, the relationship between road traffic intensity and particulate air pollution being more complex than expected.

A reliable determination of equivalent black carbon (eBC) mass concentrations derived from filter absorption photometers (FAPs) measurements depends on the appropriate quantification of the mass absorption cross-section (MAC) for converting the absorption coefficient (babs) to eBC. This study investigates the spatial–temporal variability of the MAC obtained from simultaneous elemental carbon (EC) and babs measurements performed at 22 sites. We compared different methodologies for retrieving eBC integrating different options for calculating MAC including: locally derived, median value calculated from 22 sites, and site-specific rolling MAC. The eBC concentrations that underwent correction using these methods were identified as LeBC (local MAC), MeBC (median MAC), and ReBC (Rolling MAC) respectively. Pronounced differences (up to more than 50 %) were observed between eBC as directly provided by FAPs (NeBC; Nominal instrumental MAC) and ReBC due to the differences observed between the experimental and nominal MAC values. The median MAC was 7.8 ± 3.4 m2 g-1 from 12 aethalometers at 880 nm, and 10.6 ± 4.7 m2 g-1 from 10 MAAPs at 637 nm. The experimental MAC showed significant site and seasonal dependencies, with heterogeneous patterns between summer and winter in different regions. In addition, long-term trend analysis revealed statistically significant (s.s.) decreasing trends in EC. Interestingly, we showed that the corresponding corrected eBC trends are not independent of the way eBC is calculated due to the variability of MAC. NeBC and EC decreasing trends were consistent at sites with no significant trend in experimental MAC. Conversely, where MAC showed s.s. trend, the NeBC and EC trends were not consistent while ReBC concentration followed the same pattern as EC. These results underscore the importance of accounting for MAC variations when deriving eBC measurements from FAPs and emphasize the necessity of incorporating EC observations to constrain the uncertainty associated with eBC.

Ultrafine particles (UFP, those with diameters ≤ 100 nm), have been reported to potentially penetrate deeply into the respiratory system, translocate through the alveoli, and affect various organs, potentially correlating with increased mortality. The aim of this study is to assess long-term trends (5–11 years) in mostly urban UFP concentrations based on measurements of particle number size distributions (PNSD). Additionally, concentrations of other pollutants and meteorological variables were evaluated to support the interpretations. PNSD datasets from 12 urban background (UB), 5 traffic (TR), 3 suburban background (SUB) and 1 regional background (RB) sites in 15 European cities and 1 in the USA were evaluated. The non-parametric Theil-Sen’s method was used to detect monotonic trends. Meta-analyses were carried out to assess the overall trends and those for different environments. The results showed significant decreases in NO, NO2, BC, CO, and particle concentrations in the Aitken (25–100 nm) and the Accumulation (100–800 nm) modes, suggesting a positive impact of the implementation of EURO 5/V and 6/VI vehicle standards on European air quality. The growing use of Diesel Particle Filters (DPFs) might also have clearly reduced exhaust emissions of BC, PM, and the Aitken and Accumulation mode particles. However, as reported by prior studies, there remains an issue of poor control of Nucleation mode particles (smaller than 25 nm), which are not fully reduced with current DPFs, without emission controls for semi-volatile organic compounds, and might have different origins than road traffic. Thus, contrasting trends for Nucleation mode particles were obtained across the cities studied. This mode also affected the UFP and total PNC trends because of the high proportion of Nucleation mode particles in both concentration ranges. It was also found that the urban temperature increasing trends might have also influenced those of PNC, Nucleation and Aitken modes.

Abstract Background Associations between air temperature and mortality have been consistently observed in Europe and the United States; however, there is a lack of studies for Asian countries. Our study investigated the association between air temperature and cardio-respiratory mortality in the urban area of Beijing, China. Methods Death counts for cardiovascular and respiratory diseases for adult residents (≥15 years), meteorological parameters and concentrations of particulate air pollution were obtained from January 2003 to August 2005. The effects of two-day and 15-day average temperatures were estimated by Poisson regression models, controlling for time trend, relative humidity and other confounders if necessary. Effects were explored for warm (April to September) and cold periods (October to March) separately. The lagged effects of daily temperature were investigated by polynomial distributed lag (PDL) models. Results We observed a J-shaped exposure-response function only for 15-day average temperature and respiratory mortality in the warm period, with 21.3°C as the threshold temperature. All other exposure-response functions could be considered as linear. In the warm period, a 5°C increase of two-day average temperature was associated with a RR of 1.098 (95% confidence interval (95%CI): 1.057-1.140) for cardiovascular and 1.134 (95%CI: 1.050-1.224) for respiratory mortality; a 5°C decrease of 15-day average temperature was associated with a RR of 1.040 (95%CI: 0.990-1.093) for cardiovascular mortality. In the cold period, a 5°C increase of two-day average temperature was associated with a RR of 1.149 (95%CI: 1.078-1.224) for respiratory mortality; a 5°C decrease of 15-day average temperature was associated with a RR of 1.057 (95%CI: 1.022-1.094) for cardiovascular mortality. The effects remained robust after considering particles as additional confounders. Conclusions Both increases and decreases in air temperature are associated with an increased risk of cardiovascular mortality. The effects of heat were immediate while the ones of cold became predominant with longer time lags. Increases in air temperature are also associated with an immediate increased risk of respiratory mortality.

Atmospheric aerosol particles are a complex combination of primary emitted sources (biogenic and anthropogenic) and secondary aerosol resulting from aging processes such as condensation, coagulation, and cloud processing. To better understand their sources, investigations have been focused on urban areas in the past, whereas rural-background stations are normally less impacted by surrounding anthropogenic sources. Therefore, they are predisposed for studying the impact of long-range transport of anthropogenic aerosols. Here, the chemical composition and organic aerosol (OA) sources of submicron aerosol particles measured by an aerosol chemical speciation monitor (ACSM) and a multi-angle absorption photometer (MAAP) were investigated at Melpitz from September 2016 to August 2017. The location of the station at the frontier between western and eastern Europe makes it the ideal place to investigate the impact of long-range transport over Europe. Indeed, the station is under the influence of less polluted air masses from westerly directions and more polluted continental air masses from eastern Europe. The OA dominated the submicron particle mass concentration and showed strong seasonal variability ranging from 39 % (in winter) to 58 % (in summer). It was followed by sulfate (15 % and 20 %) and nitrate (24 % and 11 %). The OA source identification was performed using the rolling positive matrix factorization (PMF) approach to account for the potential temporal changes in the source profile. It was possible to split OA into five factors with a distinct temporal variability and mass spectral signature. Three were associated with anthropogenic primary OA (POA) sources: hydrocarbon-like OA (HOA; 5.2 % of OA mass in winter and 6.8 % in summer), biomass burning OA (BBOA; 10.6 % and 6.1 %) and coal combustion OA (CCOA; 23 % and 8.7 %). Another two are secondary and processed oxygenated OA (OOA) sources: less oxidized OOA (LO-OOA; 28.4 % and 36.7 %) and more oxidized OOA (MO-OOA; 32.8 % and 41.8 %). Since equivalent black carbon (eBC) was clearly associated with the identified POA factors (sum of HOA, BBOA, and CCOA; R2= 0. 87), eBC's contribution to each of the POA factors was achieved using a multilinear regression model. Consequently, CCOA represented the main anthropogenic sources of carbonaceous aerosol (sum of OA and eBC) not only during winter (56 % of POA in winter) but also in summer (13 % of POA in summer), followed by BBOA (29 % and 69 % of POA in winter and summer, respectively) and HOA (15 % and 18 % of POA in winter and summer, respectively). A seasonal air mass cluster analysis was used to understand the geographical origins of the different aerosol types and showed that during both winter and summer time, PM1 (PM with an aerodynamic diameter smaller than 1 µm) air masses with eastern influence were always associated with the highest mass concentration and the highest coal combustion fraction. Since during wintertime CCOA is a combination of domestic heating and power plant emissions, the summer contribution of CCOA emphasizes the critical importance of coal power plant emissions to rural-background aerosols and its impact on air quality, through long-range transportation.

Anthropogenic and natural emissions contribute to enhanced concentrations of aerosols in the Arctic winter and early spring, with most attention being paid to anthropogenic aerosols that contribute to so-called Arctic haze. Less-well-studied wintertime sea-spray aerosols (SSAs) under Arctic haze conditions are the focus of this study, since they can make an important contribution to wintertime Arctic aerosol abundances. Analysis of field campaign data shows evidence for enhanced local sources of SSAs, including marine organics at Utqiaġvik (formerly known as Barrow) in northern Alaska, United States, during winter 2014. Models tend to underestimate sub-micron SSAs and overestimate super-micron SSAs in the Arctic during winter, including the base version of the Weather Research Forecast coupled with Chemistry (WRF-Chem) model used here, which includes a widely used SSA source function based on Gong et al. (1997). Quasi-hemispheric simulations for winter 2014 including updated wind speed and sea-surface temperature (SST) SSA emission dependencies and sources of marine sea-salt organics and sea-salt sulfate lead to significantly improved model performance compared to observations at remote Arctic sites, notably for coarse-mode sodium and chloride, which are reduced. The improved model also simulates more realistic contributions of SSAs to inorganic aerosols at different sites, ranging from 20 %–93 % in the observations. Two-thirds of the improved model performance is from the inclusion of the dependence on SSTs. The simulation of nitrate aerosols is also improved due to less heterogeneous uptake of nitric acid on SSAs in the coarse mode and related increases in fine-mode nitrate. This highlights the importance of interactions between natural SSAs and inorganic anthropogenic aerosols that contribute to Arctic haze. Simulation of organic aerosols and the fraction of sea-salt sulfate are also improved compared to observations. However, the model underestimates episodes with elevated observed concentrations of SSA components and sub-micron non-sea-salt sulfate at some Arctic sites, notably at Utqiaġvik. Possible reasons are explored in higher-resolution runs over northern Alaska for periods corresponding to the Utqiaġvik field campaign in January and February 2014. The addition of a local source of sea-salt marine organics, based on the campaign data, increases modelled organic aerosols over northern Alaska. However, comparison with previous available data suggests that local natural sources from open leads, as well as local anthropogenic sources, are underestimated in the model. Missing local anthropogenic sources may also explain the low modelled (sub-micron) non-sea-salt sulfate at Utqiaġvik. The introduction of a higher wind speed dependence for sub-micron SSA emissions, also based on Arctic data, reduces biases in modelled sub-micron SSAs, while sea-ice fractions, including open leads, are shown to be an important factor controlling modelled super-micron, rather than sub-micron, SSAs over the north coast of Alaska. The regional results presented here show that modelled SSAs are more sensitive to wind speed dependence but that realistic modelling of sea-ice distributions is needed for the simulation of local SSAs, including marine organics. This study supports findings from the Utqiaġvik field campaign that open leads are the primary source of fresh and aged SSAs, including marine organic aerosols, during wintertime at Utqiaġvik; these findings do not suggest an influence from blowing snow and frost flowers. To improve model simulations of Arctic wintertime aerosols, new field data on processes that influence wintertime SSA production, in particular for fine-mode aerosols, are needed as is improved understanding about possible local anthropogenic sources.

The interaction between water vapor and aerosol nanoparticles is important in atmospheric processes. Hygroscopicity of sub-10 nm organic nanoparticles and their concentration-dependent thermodynamic properties (e.g., water activity) in the highly supersaturated concentration range are, however, scarcely available. Here we investigate the size dependence of hygroscopicity of organics (i.e., levoglucosan, D-glucose) in dry particle diameter down to 6 nm using a nano-hygroscopicity tandem differential mobility analyzer (nano-HTDMA). Our results show that there is only weak size-dependent hygroscopic growth of both levoglucosan and D-glucose nanoparticles with diameters down to 20 nm. In the diameter range smaller than 20 nm (down to 6 nm), we observed strong size-dependent hygroscopic growth for D-glucose nanoparticles. The hygroscopic growth factors cannot be determined for levoglucosan below 20 nm due to its evaporation. In addition, we compare hygroscopicity measurements for levoglucosan and D-glucose nanoparticles with E-AIM (standard UNIFAC – functional group activity coefficients), the ideal solution theory, and differential Köhler analysis (DKA) predictions. The ideal solution theory describes the measured hygroscopic growth factors of levoglucosan with diameters down to 20 nm and D-glucose nanoparticles with diameters larger than 60 nm, while E-AIM (standard UNIFAC) can successfully predict the growth factors of D-glucose nanoparticles with diameters from 100 down to 6 nm at RH above 88 %–40 % (e.g., at RH above 88 % for 100 nm D-glucose, at RH above 40 % for 6 nm D-glucose). The use of the DKA method leads to good agreement with measured hygroscopic growth factors of D-glucose aerosol nanoparticles with diameters from 100 down to 6 nm. Predicted water activity for these aqueous organic solutions (i.e., levoglucosan, D-glucose) from different parameterization methods agrees well with observations in the low solute concentration range (< 20 mol kg−1) and starts to deviate from observations in the high solute concentration (> 20 mol kg−1).

Objectives: This paper presents the study design of the Berlin-Brandenburg Air study (BEAR-study). We measure air quality in Berlin and Brandenburg before and after the relocation of aircraft (AC) traffic from Tegel (TXL) airport to the new Berlin-Brandenburg airport (BER) and investigate the association of AC-related ultrafine particles (UFP) with health outcomes in schoolchildren.Methods: The BEAR-study is a natural experiment examining schoolchildren attending schools near TXL and BER airports, and in control areas (CA) away from both airports and associated air corridors. Each child undergoes repeated school-based health-examinations. Total particle number concentration (PNC) and meteorological parameters are continuously monitored. Submicrometer particle number size distribution, equivalent black carbon, and gas-phase pollutants are collected from long-term air quality monitoring stations. Daily source-specific UFP concentrations are modeled. We will analyze short-term effects of UFP on respiratory, cardiovascular, and neurocognitive outcomes, as well as medium and long-term effects on lung growth and cognitive development.Results: We examined 1,070 children (as of 30 November 2022) from 16 schools in Berlin and Brandenburg.Conclusion: The BEAR study increases the understanding of how AC-related UFP affect children’s health.

In this work, new particle formation events (NPFs) occurring at two locations in southern Italy, the urban background site of Lecce (ECO station) and the coastal site of Lamezia Terme (LMT station), are identified and analyzed. The study aims to compare the properties of NPF events at the two sites, located 225 km away from each other and characterized by marked differences in terms of emission sources and local weather dynamics. Continuous measurements of particle number size distributions, in the size range from 10 to 800 m, were performed at both sites by a mobility particle size spectrometer (MPSS). The occurrence of NPF events, observed throughout the study period that lasted 5 years, produced different results in terms of frequency of occurrence: 25 % of the days at ECO and 9 % at LMT. NPF events showed seasonal patterns: higher frequency during spring and summer at the urban background site and the autumn–winter period at the coastal site. Some of these events happened simultaneously at both sites, indicating the occurrence of the nucleation process on a large spatial scale. Cluster analysis of 72 h back trajectories showed that during the NPF events the two stations were influenced by similar air masses, most of which originated from the north-western direction. Local meteorological conditions characterized by high pressure, with a prevalence of clear skies, low levels of relative humidity (RH < 52 %), and moderate winds (3–4 m s−1) dominated the NPF events at both sites. Notable differences were observed in SO2 and PM2.5 concentrations and H2SO4 proxy levels, resulting in ∼65 %, ∼80 %, and 50 % lower levels at LMT compared to ECO, respectively. It is likely that the lower level of that which is recognized as one of the main gas precursors involved in the nucleation process could be responsible for the smaller NPF frequency of occurrence (∼60 % less than ECO) observed in LMT.

Dimethyl sulfide (DMS) is the primary natural contributor to the atmospheric sulfur burden. Observations concerning the fate of DMS oxidation products after long-range transport in the remote free troposphere are, however, sparse. Here we present quantitative chemical ionization mass spectrometric measurements of DMS and its oxidation products sulfuric acid (H2SO4), methanesulfonic acid (MSA), dimethylsulfoxide (DMSO), dimethylsulfone (DMSO2), methanesulfinic acid (MSIA), methyl thioformate (MTF), methanesulfenic acid (MSEA, CH3SOH), and a compound of the likely structure CH3S(O)2OOH in the gas phase, as well as measurements of the sulfate and methanesulfonate aerosol mass fractions. The measurements were performed at the Global Atmosphere Watch (GAW) station Chacaltaya in the Bolivian Andes located at 5240 m above sea level (a.s.l.). DMS and DMS oxidation products are brought to the Andean high-altitude station by Pacific air masses during the dry season after convective lifting over the remote Pacific ocean to 6000–8000 m a.s.l. and subsequent long-range transport in the free troposphere (FT). Most of the DMS reaching the station is already converted to the rather unreactive sulfur reservoirs DMSO2 in the gas phase and methanesulfonate (MS−) in the particle phase, which carried nearly equal amounts of sulfur to the station. The particulate sulfate at Chacaltaya is however dominated by regional volcanic emissions during the time of the measurement and not significantly affected by the marine air masses. In one of the FT events, even some DMS was observed next to reactive intermediates such as methyl thioformate, dimethylsulfoxide, and methanesulfinic acid. Also for this event, back trajectory calculations show that the air masses came from above the ocean (distance >330 km) with no local surface contacts. This study demonstrates the potential impact of marine DMS emissions on the availability of sulfur-containing vapors in the remote free troposphere far away from the ocean.

The Arctic environment is rapidly changing due to accelerated warming in the region. The warming trend is driving a decline in sea ice extent, which thereby enhances feedback loops in the surface energy budget in the Arctic. Arctic aerosols play an important role in the radiative balance and hence the climate response in the region, yet direct observations of aerosols over the Arctic Ocean are limited. In this study, we investigate the annual cycle in the aerosol particle number size distribution (PNSD), particle number concentration (PNC), and black carbon (BC) mass concentration in the central Arctic during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition. This is the first continuous, year-long data set of aerosol PNSD ever collected over the sea ice in the central Arctic Ocean. We use a k-means cluster analysis, FLEXPART simulations, and inverse modeling to evaluate seasonal patterns and the influence of different source regions on the Arctic aerosol population. Furthermore, we compare the aerosol observations to land-based sites across the Arctic, using both long-term measurements and observations during the year of the MOSAiC expedition (2019–2020), to investigate interannual variability and to give context to the aerosol characteristics from within the central Arctic. Our analysis identifies that, overall, the central Arctic exhibits typical seasonal patterns of aerosols, including anthropogenic influence from Arctic haze in winter and secondary aerosol processes in summer. The seasonal pattern corresponds to the global radiation, surface air temperature, and timing of sea ice melting/freezing, which drive changes in transport patterns and secondary aerosol processes. In winter, the Norilsk region in Russia/Siberia was the dominant source of Arctic haze signals in the PNSD and BC observations, which contributed to higher accumulation-mode PNC and BC mass concentrations in the central Arctic than at land-based observatories. We also show that the wintertime Arctic Oscillation (AO) phenomenon, which was reported to achieve a record-breaking positive phase during January–March 2020, explains the unusual timing and magnitude of Arctic haze across the Arctic region compared to longer-term observations. In summer, the aerosol PNCs of the nucleation and Aitken modes are enhanced; however, concentrations were notably lower in the central Arctic over the ice pack than at land-based sites further south. The analysis presented herein provides a current snapshot of Arctic aerosol processes in an environment that is characterized by rapid changes, which will be crucial for improving climate model predictions, understanding linkages between different environmental processes, and investigating the impacts of climate change in future Arctic aerosol studies.

Despite a large number of studies, out of all drivers of radiative forcing, the effect of aerosols has the largest uncertainty in global climate model radiative forcing estimates. There have been studies of aerosol optical properties in climate models, but the effects of particle number size distribution need a more thorough inspection. We investigated the trends and seasonality of particle number concentrations in nucleation, Aitken, and accumulation modes at 21 measurement sites in Europe and the Arctic. For 13 of those sites, with longer measurement time series, we compared the field observations with the results from five climate models, namely EC-Earth3, ECHAM-M7, ECHAM-SALSA, NorESM1.2, and UKESM1. This is the first extensive comparison of detailed aerosol size distribution trends between in situ observations from Europe and five earth system models (ESMs). We found that the trends of particle number concentrations were mostly consistent and decreasing in both measurements and models. However, for many sites, climate models showed weaker decreasing trends than the measurements. Seasonal variability in measured number concentrations, quantified by the ratio between maximum and minimum monthly number concentration, was typically stronger at northern measurement sites compared to other locations. Models had large differences in their seasonal representation, and they can be roughly divided into two categories: for EC-Earth and NorESM, the seasonal cycle was relatively similar for all sites, and for other models the pattern of seasonality varied between northern and southern sites. In addition, the variability in concentrations across sites varied between models, some having relatively similar concentrations for all sites, whereas others showed clear differences in concentrations between remote and urban sites. To conclude, although all of the model simulations had identical input data to describe anthropogenic mass emissions, trends in differently sized particles vary among the models due to assumptions in emission sizes and differences in how models treat size-dependent aerosol processes. The inter-model variability was largest in the accumulation mode, i.e. sizes which have implications for aerosol–cloud interactions. Our analysis also indicates that between models there is a large variation in efficiency of long-range transportation of aerosols to remote locations. The differences in model results are most likely due to the more complex effect of different processes instead of one specific feature (e.g. the representation of aerosol or emission size distributions). Hence, a more detailed characterization of microphysical processes and deposition processes affecting the long-range transport is needed to understand the model variability.

This study analyzed the variability of equivalent black carbon (eBC) mass concentrations and their sources in urban Europe to provide insights into the use of eBC as an advanced air quality (AQ) parameter for AQ standards. This study compiled eBC mass concentration datasets covering the period between 2006 and 2022 from 50 measurement stations, including 23 urban background (UB), 18 traffic (TR), 7 suburban (SUB), and 2 regional background (RB) sites. The results highlighted the need for the harmonization of eBC measurements to allow for direct comparisons between eBC mass concentrations measured across urban Europe. The eBC mass concentrations exhibited a decreasing trend as follows: TR > UB > SUB > RB. Furthermore, a clear decreasing trend in eBC concentrations was observed in the UB sites moving from Southern to Northern Europe. The eBC mass concentrations exhibited significant spatiotemporal heterogeneity, including marked differences in eBC mass concentration and variable contributions of pollution sources to bulk eBC between different cities. Seasonal patterns in eBC concentrations were also evident, with higher winter concentrations observed in a large proportion of cities, especially at UB and SUB sites. The contribution of eBC from fossil fuel combustion, mostly traffic (eBCT) was higher than that of residential and commercial sources (eBCRC) in all European sites studied. Nevertheless, eBCRC still had a substantial contribution to total eBC mass concentrations at a majority of the sites. eBC trend analysis revealed decreasing trends for eBCT over the last decade, while eBCRC remained relatively constant or even increased slightly in some cities.

Black carbon (BC) is a major component of submicron particulate matter (PM), with significant health and climate impacts. Many cities in emerging countries lack comprehensive knowledge about BC emissions and exposure levels. This study investigates BC concentration levels, identifies its emission sources, and characterizes the optical properties of BC at urban background sites of the two largest high-altitude Bolivian cities: La Paz (LP) (3600 m above sea level) and El Alto (EA) (4050 m a.s.l.), where atmospheric oxygen levels and intense radiation may affect BC production. The study relies on concurrent measurements of equivalent black carbon (eBC), elemental carbon (EC), and refractory black carbon (rBC) and their comparison with analogous data collected at the nearby Chacaltaya Global Atmosphere Watch Station (5240 m a.s.l). The performance of two independent source apportionment techniques was compared: a bilinear model and a least-squares multilinear regression (MLR). Maximum eBC concentrations were observed during the local dry season (LP: eBC = 1.5 ± 1.6 µ g m−3; EA: 1.9±2.0 µ g m−3). While eBC concentrations are lower at the mountain station, daily transport from urban areas is evident. Average mass absorption cross sections of 6.6–8.2 m2 g−1 were found in the urban area at 637 nm. Both source apportionment methods exhibited a reasonable level of agreement in the contribution of biomass burning (BB) to absorption. The MLR method allowed the estimation of the contribution and the source-specific optical properties for multiple sources, including open waste burning. [ABSTRACT FROM AUTHOR]

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 PN10-25, 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 PN10-25, 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 PN25-800, 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