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Abstract Atmospheric new particle formation (NPF) is a naturally occurring phenomenon, during which high concentrations of sub-10 nm particles are created through gas to particle conversion. The NPF is observed in multiple environments around the world. Although it has observable influence onto annual total and ultrafine particle number concentrations (PNC and UFP, respectively), only limited epidemiological studies have investigated whether these particles are associated with adverse health effects. One plausible reason for this limitation may be related to the absence of NPF identifiers available in UFP and PNC data sets. Until recently, the regional NPF events were usually identified manually from particle number size distribution contour plots. Identification of NPF across multi-annual and multiple station data sets remained a tedious task. In this work, we introduce a regional NPF identifier, created using an automated, machine learning based algorithm. The regional NPF event tag was created for 65 measurement sites globally, covering the period from 1996 to 2023. The discussed data set can be used in future studies related to regional NPF.

Constraining dust models to understand and quantify the effect of dust upon climate and ecosystems requires comprehensive analyses of the physiochemical properties of dust-emitting sediments in arid regions. Building upon previous studies in the Moroccan Sahara and Iceland, we analyse a diverse set of crusts and aeolian ripples (n=55) from various potential dust-emitting basins within the Mojave Desert, California, USA. Our focus is on characterizing the particle size distribution (PSD), mineralogy, aggregation/cohesion state, and Fe mode of occurrence. Our results show differences in fully and minimally dispersed PSDs, with crusts exhibiting average median diameters of 92 and 37 µm, respectively, compared to aeolian ripples with 226 and 213 µm, respectively. Mineralogical analyses unveiled strong variations between crusts and ripples, with crusts being enriched in phyllosilicates (24 % vs. 7.8 %), carbonates (6.6 % vs. 1.1 %), Na salts (7.3 % vs. 1.1 %), and zeolites (1.2 % and 0.12 %) and ripples being enriched in feldspars (48 % vs. 37 %), quartz (32 % vs. 16 %), and gypsum (4.7 % vs. 3.1 %). The size fractions from crust sediments display a homogeneous mineralogy, whereas those of aeolian ripples display more heterogeneity, mostly due to different particle aggregation. Bulk Fe content analyses indicate higher concentrations in crusts (3.0 ± 1.3 wt %) compared to ripples (1.9 ± 1.1 wt %), with similar proportions in their Fe mode of occurrence: nano-sized Fe oxides and readily exchangeable Fe represent ∼1.6 %, hematite and goethite ∼15 %, magnetite/maghemite ∼2.0 %, and structural Fe in silicates ∼80 % of the total Fe. We identified segregation patterns in the PSD and mineralogy differences in Na salt content within the Mojave basins, which can be explained by sediment transportation dynamics and precipitates due to groundwater table fluctuations described in previous studies in the region. Mojave Desert crusts show similarities with previously sampled crusts in the Moroccan Sahara in terms of the PSD and readily exchangeable Fe yet exhibit substantial differences in mineralogical composition, which should significantly influence the characteristic of the emitted dust particles.

Characterising the physico-chemical properties of dust-emitting sediments in arid regions is fundamental to understanding the effects of dust on climate and ecosystems. However, knowledge regarding high-latitude dust (HLD) remains limited. This study focuses on analysing the particle size distribution (PSD), mineralogy, cohesion, iron (Fe) mode of occurrence, and visible–near infrared (VNIR) reflectance spectra of dust-emitting sediments from dust hotspots in Iceland (HLD region). Extensive analysis was conducted on samples of top sediments, sediments, and aeolian ripples collected from seven dust sources, with particular emphasis on the Jökulsá basin, encompassing the desert of Dyngjunsandur. Both fully and minimally dispersed PSDs and their respective mass median particle diameters revealed remarkable similarities (56 ± 69 and 55 ± 62 µm, respectively). Mineralogical analyses indicated the prevalence of amorphous phases (68 ± 26 %), feldspars (17 ± 13 %), and pyroxenes (9.3 ± 7.2 %), consistent with thorough analyses of VNIR reflectance spectra. The Fe content reached 9.5 ± 0.40 wt %, predominantly within silicate structures (80 ± 6.3 %), complemented by magnetite (16 ± 5.5 %), hematite/goethite (4.5 ± 2.7 %), and readily exchangeable Fe ions or Fe nano-oxides (1.6 ± 0.63 %). Icelandic top sediments exhibited coarser PSDs compared to the high dust-emitting crusts from mid-latitude arid regions, distinctive mineralogy, and a 3-fold bulk Fe content, with a significant presence of magnetite. The congruence between fully and minimally dispersed PSDs underscores reduced particle aggregation and cohesion of Icelandic top sediments, suggesting that aerodynamic entrainment of dust could also play a role upon emission in this region, alongside saltation bombardment. The extensive analysis in Dyngjusandur enabled the development of a conceptual model to encapsulate Iceland's rapidly evolving high dust-emitting environments.

The rapid expansion of the aviation sector raises concerns about air quality impacts within and around airports. Ultrafine particles (UFP, diameter 2-fold) of Fe, Al, Cr, Cu, Mo, Mn, Pb, Ti, and Sb at the airport compared to the UB, with Al exhibiting the most pronounced disparity. Generally, PAH levels were low at both sites, although concentrations were higher at the airport relative to the UB. Overall, this study provides a comprehensive understanding of UFP within a major European airport, identifying the different sources contributing to PNC and PNSD.

This study analyses three extreme ozone (O3) episodes that occurred in Barcelona (NE Spain) during the summers of 2015, 2018, and 2019. These episodes exceeded the EU's hourly information threshold (180 µg m−3) for the first time since at least the year 2000, raising concerns due to Barcelona's large population. By employing experimental data and various modelling tools, our main objective is to elucidate the underlying phenomena of these recent O3 episodes and improve predictive capabilities. The findings indicate that the factors contributing to these occurrences are largely consistent across episodes. These factors, with estimated O3 contributions specified for particular instances, comprise (i) initial O3 accumulation in surrounding coastal areas; (ii) weekend occurrence, accompanied by the corresponding weekend effect (+15 µg m−3); and (iii) the prevalence of Tramontana meteorological conditions during above-normal temperatures, which (iv) force the convergence of multiregional polluted air masses to the city (+45–65 µg m−3). Major source areas include regions of southern France through the Gulf of Lion, the interior of the Mediterranean, and eastern Spanish coastal regions, including Barcelona's pollution plume. Some of these factors, which may manifest in the days preceding the episodes, are observable or can be anticipated. This study enhances understanding of the mechanisms driving extreme O3 episodes recently observed in Barcelona and provides valuable insights for prediction.

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.

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.

The European Commission Directive, 1999/30/EC, approved on the 22nd of April 1999, on atmospheric particles establishes a standard that is more stringent than the current one. This Directive proposes the monitoring of particles lower than 10 μm (PM10, thoracic particles) based on health impact criteria. The proposed EC limits are 40 μgPM10.m-3 and 20 μgPM10.m-3 as annual means in 2005 and 2010, respectively. In accordance with the European Commission (EC), the future PM10 limits will be revised in 2003 if the European States can demonstrate that the exceedances of the new limits are attributed to natural inputs. The exceedances due to natural inputs are more frequent in Mediterranean countries due to the re-suspension of natural soil particles and to the higher frequency of Saharan air mass intrusions. This study summarises the preliminary results obtained from two research projects in Spain focused on: 1) establishing the criteria for the discrimination of natural/anthropogenic inputs of PM10; 2) identifying the events when the proposed limits are exceeded by natural inputs and 3) determining the most suitable monitoring parameter, PM10 or PM2.5, in order to avoid natural interference. Given the importance of the ceramic industry in Castelló, special attention will be placed on the preliminary results obtained this area.La Directiva de la comisión Europea, 1999/30/CE, aprobada el 22 de Abril de 1999, referida a partículas atmosféricas en suspensión, establece una normativa más estricta que la vigente. Esta normativa propone el control de las partículas inferiores a 10 μm (PM10, partículas torácicas) basándose en criterios de impacto en la salud. Según esta directiva no se podrán superar medias diarias anuales de 40 μgPM10.m-3 en el 2005 y de 20 μgPM10.m-3 en el 2010. La directiva contempla la revisión de los límites normativos y de los parámetros de control en el 2003, pudiendo variar estos en el caso de que los Estados miembros demuestren que los rebasamientos de los nuevos límites normativos se deban a causas naturales. Estas superaciones por causas naturales son más frecuentes en los países del área Mediterránea debido a la resuspensión de partículas naturales y la mayor frecuencia de intrusiones de masas de aire del Sahara. El presente trabajo presenta los resultados preliminares de dos proyectos de investigación, desarrollados en el territorio español, cuyos objetivos principales son: 1) establecer los criterios para la discriminación de aportes naturales/antropogénicos de PM10; 2) identificar cuando las superaciones de los limites de PM10 se superan por causas naturales y 3) determinar la conveniencia de medir PM2.5 o PM10 para evitar la interferencia de aerosoles naturales en el PM10. En este trabajo se van a resaltar los resultados obtenidos en el área de Castelló, debido a la gran industria cerámica presente en esta zona, con objeto de estudiar el posible impacto de la nueva Directiva europea en la industria cerámica.

Detailed knowledge on the formation of new aerosol particles in the atmosphere from precursor gases, and their subsequent growth, commonly known as new particle formation (NPF) events, is one of the largest challenges in atmospheric aerosol science. High pre-existing particle loadings are expected to suppress the formation of new atmospheric aerosol particles due to high coagulation and condensation (CS) sinks. However, NPF events are regularly observed in conditions with high concentrations of pre-existing particles and even during intense desert dust intrusions that imply discrepancies between the observations and theory. In this study, we present a multi-site analysis of the occurrence of NPF events under the presence of desert dust particles in dust-influenced areas. Characterization of NPF events at five different locations highly influenced by desert dust outbreaks was done under dusty and non-dusty conditions using continuous measurements of aerosol size distribution in both fine and coarse size fractions. Contrary to common thought, our results show that the occurrence of NPF events is highly frequent during desert dust outbreaks, showing that NPF event frequencies during dusty conditions are similar to those observed during non-dusty conditions. Furthermore, our results show that NPF events also occur during intense desert dust outbreaks at all the studied sites, even at remote sites where the amounts of precursor vapours are expected to be low. Our results show that the condensation sink associated with coarse particles (CSC) represents up to the 60 % of the total CS during dusty conditions, which highlights the importance of considering coarse-fraction particles for NPF studies in desert-dust-influenced areas. However, we did not find a clear pattern of the effect of desert dust outbreaks on the strength of NPF events, with differences from site to site. The particle growth rate (GR) did not present a clear dependence on the CS during dusty and non-dusty conditions. This result, together with the fact that desert dust has different effects on the growth and formation rates at each site, suggests different formation and growth mechanisms at each site between dusty and non-dusty conditions, probably due to differences in precursor vapours' origins and concentrations as well as changes in the oxidative capacity of pre-existing particles and their effectiveness acting as CS. Further investigation based on multiplatform measurement campaigns and chamber experiments with state-of-the-art gaseous and particulate physical and chemical properties measurements is needed to better understand the role of catalyst components present in desert dust particles in NPF. Finally, our results reveal a significant impact of NPF events on the cloud condensation nuclei (CCN) budget during desert dust outbreaks at the studied sites. Therefore, since desert dust contributes to a major fraction of the global aerosol mass load, and since there is a foreseeable increase in the frequency, duration and intensity of desert dust episodes due to climate change, it is imperative to improve our understanding of the effect of desert dust outbreaks on NPF and the CCN budget for better climate change prediction.

The effects of desert dust upon climate and ecosystems depend strongly on its particle size and size-resolved mineralogical composition. However, there is very limited quantitative knowledge on the particle size and composition of the parent sediments along with their variability within dust-source regions, particularly in dust emission hotspots. The lower Drâa Valley, an inland drainage basin and dust hotspot region located in the Moroccan Sahara, was chosen for a comprehensive analysis of sediment particle size and mineralogy. Different sediment type samples (n= 42) were collected, including paleo-sediments, paved surfaces, crusts, and dunes, and analysed for particle-size distribution (minimally and fully dispersed samples) and mineralogy. Furthermore, Fe sequential wet extraction was carried out to characterise the modes of occurrence of Fe, including Fe in Fe (oxyhydr)oxides, mainly from goethite and hematite, which are key to dust radiative effects; the poorly crystalline pool of Fe (readily exchangeable ionic Fe and Fe in nano-Fe oxides), relevant to dust impacts upon ocean biogeochemistry; and structural Fe. Results yield a conceptual model where both particle size and mineralogy are segregated by transport and deposition of sediments during runoff of water across the basin and by the precipitation of salts, which causes a sedimentary fractionation. The proportion of coarser particles enriched in quartz is higher in the highlands, while that of finer particles rich in clay, carbonates, and Fe oxides is higher in the lowland dust emission hotspots. There, when water ponds and evaporates, secondary carbonates and salts precipitate, and the clays are enriched in readily exchangeable ionic Fe, due to sorption of dissolved Fe by illite. The results differ from currently available mineralogical atlases and highlight the need for observationally constrained global high-resolution mineralogical data for mineral-speciated dust modelling. The dataset obtained represents an important resource for future evaluation of surface mineralogy retrievals from spaceborne spectroscopy.

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.

This study addressed the scarcity of NH3 measurements in urban Europe and the diverse monitoring protocols, hindering direct data comparison. Sixty-nine datasets from Finland, France, Italy, Spain, and the UK across various site types, including industrial (IND, 8), traffic (TR, 12), urban (UB, 22), suburban (SUB, 12), and regional background (RB, 15), are analyzed to this study. Among these, 26 sites provided 5, or more, years of data for time series analysis. Despite varied protocols, necessitating future harmonization, the average NH3 concentration across sites reached 8.0 ± 8.9 μg/m3. Excluding farming/agricultural hotspots (FAHs), IND and TR sites had the highest concentrations (4.7 ± 3.2 and 4.5 ± 1.0 μg/m3), followed by UB, SUB, and RB sites (3.3 ± 1.5, 2.7 ± 1.3, and 1.0 ± 0.3 μg/m3, respectively) indicating that industrial, traffic, and other urban sources were primary contributors to NH3 outside FAH regions. When referring exclusively to the FAHs, concentrations ranged from 10.0 ± 2.3 to 15.6 ± 17.2 μg/m3, with the highest concentrations being reached in RB sites close to the farming and agricultural sources, and that, on average for FAHs there is a decreasing NH3 concentration gradient towards the city. Time trends showed that over half of the sites (18/26) observed statistically significant trends. Approximately 50 % of UB and TR sites showed a decreasing trend, while 30 % an increasing one. Meta-analysis revealed a small insignificant decreasing trend for non-FAH RB sites. In FAHs, there was a significant upward trend at a rate of 3.51[0.45,6.57]%/yr. Seasonal patterns of NH3 concentrations varied, with urban areas experiencing fluctuations influenced by surrounding emissions, particularly in FAHs. Diel variation showed differing patterns at urban monitoring sites, all with higher daytime concentrations, but with variations in peak times depending on major emission sources and meteorological patterns. These results offer valuable insights into the spatio-temporal patterns of gas-phase NH3 concentrations in urban Europe, contributing to future efforts in benchmarking NH3 pollution control in urban areas.

Aerosols are one of the most important pollutants in the atmosphere and have been monitored for the past few decades by remote sensing and in situ observation platforms to assess the effectiveness of government-managed reduction emission policies and assess their impact on the radiative budget of the Earth's atmosphere. In fact, aerosols can directly modulate incoming short-wave solar radiation and outgoing long-wave radiation and indirectly influence cloud formation, lifetime, and precipitation. In this study, we quantitatively evaluated long-term temporal trends and seasonal variability from a climatological point of view of the optical and microphysical properties of atmospheric particulate matter at the Universitat Politècnica de Catalunya (UPC), Barcelona, Spain, over the past 17 years, through a synergy of lidar, sun photometer, and in situ concentration measurements. Interannual temporal changes in aerosol optical and microphysical properties are evaluated through the seasonal Mann–Kendall test. Long-term trends in the optical depth of the recovered aerosol; the Ångström exponent (AE); and the concentrations of PM10, PM2.5, and PM1 reveal that emission reduction policies implemented in the past decades were effective in improving air quality, with consistent drops in PM concentrations and optical depth of aerosols. The seasonal analysis of the 17-year average vertically resolved aerosol profiles obtained from lidar observations shows that during summer the aerosol layer can be found up to an altitude of 5 km, after a sharp decay in the first kilometer. In contrast, during the other seasons, the backscatter profiles fit a pronounced exponential decay well with a well-defined scale height. Long-range transport, especially dust outbreaks from the Sahara, is likely to occur throughout the year. During winter, the dust aerosol layers are floating above the boundary layer, while during the other seasons they can penetrate the layer. The analysis also revealed that intense, short-duration pollution events during winter, associated with dust outbreaks, have become more frequent and intense since 2016. This study sheds some light on the meteorological processes and conditions that can lead to the formation of haze and helps decision makers adopt mitigation strategies to preserve large metropolitan areas in the Mediterranean basin.

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.

The particle size distribution (PSD) of mineral dust has a strong effect on the impacts of dust on climate. However, our understanding of the emitted dust PSD, including its variability and the fraction of super-coarse dust (diameter >10 µm), remains limited. Here, we provide new insights into the size-resolved dust emission process based on a field campaign performed in the Moroccan Sahara in September 2019 in the context of the FRontiers in dust minerAloGical coMposition and its Effects upoN climaTe (FRAGMENT) project. The obtained dust concentration and diffusive flux PSDs show significant dependencies upon the friction velocity (u*), wind direction and type of event (regular events versus haboob events). For instance, the number fraction of sub-micrometre particles increases with u*, along with a large decrease in the mass fraction of super-coarse dust. We identify dry deposition, which is modulated by u* and fetch length, as a potential cause for this PSD variability. Using a resistance model constrained with field observations to estimate the dry deposition flux and thereby also the emitted dust flux, we show that deposition could represent up to ∼90 % of the emission of super-coarse particles (>10 µm) and up to ∼65 % of the emission of particles as small as ∼5 µm in diameter. Importantly, removing the deposition component significantly reduces the variability with u* in the PSD of the emitted dust flux compared with the diffusive flux, particularly for super-coarse dust. The differences between regular and haboob event concentration and diffusive flux PSDs are suspected to result from a smaller and variable dust source fetch during the haboob events, and/or an increased resistance of soil aggregates to fragmentation associated with the observed increase in relative humidity along the haboob outflow. Finally, compared to the invariant emitted dust flux PSD estimated based on brittle fragmentation theory, we obtain a substantially higher proportion of super-micrometre particles in the dust flux. Overall, our results suggest that dry deposition needs to be adequately considered to estimate the emitted PSD, even in studies limited to the fine and coarse size ranges ( µm).

Black carbon (BC) has received increasing attention from researchers due to its adverse health effects. However, in-situ BC measurements are often not included as a regulated variable in air quality monitoring networks. Machine learning (ML) models have been studied extensively to serve as virtual sensors to complement the reference instruments. This study evaluates and compares three white-box (WB) and four black-box (BB) ML models to estimate BC concentrations, with the focus to show their transferability and interpretability. We train the models with the long-term air pollutant and weather measurements in Barcelona urban background site, and test them in other European urban and traffic sites. Despite the difference in geographical locations and measurement sites, BC correlates the strongest with particle number concentration of accumulation mode (PNacc, r = 0.73–0.85) and nitrogen dioxide (NO2, r = 0.68–0.85) and the weakest with meteorological parameters. Due to its similarity of correlation behaviour, the ML models trained in Barcelona performs prominently at the traffic site in Helsinki (R2 = 0.80–0.86; mean absolute error MAE = 3.90–4.73 %) and at the urban background site in Dresden (R2 = 0.79–0.84; MAE = 4.23–4.82 %). WB models appear to explain less variability of BC than BB models, long short-term memory (LSTM) model of which outperforms the rest of the models. In terms of interpretability, we adopt several methods for individual model to quantify and normalize the relative importance of each input feature. The overall static relative importance commonly used for WB models demonstrate varying results from the dynamic values utilized to show local contribution used for BB models. PNacc and NO2 on average have the strongest absolute static contribution; however, they simultaneously impact the estimation positively and negatively at different sites. This comprehensive analysis demonstrates that the possibility of these interpretable air pollutant ML models to be transfered across space and time.

For a Positive Matrix Factorization (PMF) aerosol source apportionment (SA) studies there is no standard procedure to select the most appropriate chemical components to be included in the input dataset for a given site typology, nor specific recommendations in this direction. However, these choices are crucial for the final SA outputs not only in terms of number of sources identified but also, and consequently, in the source contributions estimates. In fact, PMF tends to reproduce most of PM mass measured independently and introduced as a total variable in the input data, regardless of the percentage of PM mass which has been chemically characterized, so that the lack of some specific source tracers (e.g. levoglucosan) can potentially affect the results of the whole source apportionment study. The present study elaborates further on the same concept, evaluating quantitatively the impact of lacking specific sources’ tracers on the whole source apportionment, both in terms of identified sources and source contributions. This work aims to provide first recommendations on the most suitable and critical components to be included in PMF analyses in order to reduce PMF output uncertainty as much as possible, and better represent the most commons PM sources observed in many sites in Western countries. To this aim, we performed three sensitivity analyses on three different datasets across EU, including extended sets of organic tracers, in order to cover different types of urban conditions (Mediterranean, Continental, and Alpine), source types, and PM fractions. Our findings reveal that the vehicle exhaust source resulted to be less sensitive to the choice of analytes, although source contributions estimates can deviate significantly up to 44 %. On the other hand, for the detection of the non-exhaust one is clearly necessary to analyze specific inorganic elements. The choice of not analysing non-polar organics likely causes the loss of separation of exhaust and non-exhaust factors, thus obtaining a unique road traffic source, which provokes a significant bias of total contribution. Levoglucosan was, in most cases, crucial to identify biomass burning contributions in Milan and in Barcelona, in spite of the presence of PAHs in Barcelona, while for the case of Grenoble, even discarding levoglucosan, the presence of PAHs allowed identifying the BB factor. Modifying the rest of analytes provoke a systematic underestimation of biomass burning source contributions. SIA factors resulted to be generally overestimated with respect to the base case analysis, also in the case that ions were not included in the PMF analysis. Trace elements were crucial to identify shipping emissions (V and Ni) and industrial sources (Pb, Ni, Br, Zn, Mn, Cd and As). When changing the rest of input variables, the uncertainty was narrow for shipping but large for industrial processes. Major and trace elements were also crucial to identify the mineral/soil factor at all cities. Biogenic SOA and Anthropogenic SOA factors were sensitive to the presence of their molecular tracers, since the availability of OC alone is unable to separate a SOA factor. Arabitol and sorbitol were crucial to detecting fungal spores while odd number of higher alkanes (C27 to C31) for plant debris.

Understanding the atmospheric processes involving carbonaceous aerosols (CAs) is crucial for assessing air pollution impacts on human health and climate. The sources and formation mechanisms of CAs are not well understood, making it challenging to quantify impacts in models. Studies suggest residential wood combustion (RWC) and traffic significantly contribute to CAs in Europe’s urban and rural areas.Here, we used an atmospheric chemistry model (MONARCH) and three different emission inventories (two versions of the European-scale emission inventory CAMS-REG_v4 and the HERMESv3 detailed national inventory for Spain) to assess the uncertainties in CAs simulation and source allocation (from traffic, RWC, shipping, fires and others) in Northeast Spain. For this, black carbon (BC) and organic aerosol (OA) measurements performed at three supersites representing different environments (urban, regional and remote) were used. Our findings show the importance of model resolution and detailed emission input data in accurately reproducing BC/OA observations. Even though emissions of total particulate matter are rather consistent between inventories in Spain, we found discrepancies between them mainly related to the spatiotemporal disaggregation (particularly relevant for traffic and RWC) and the treatment of the condensable fraction of CAs in RWC (changes in the speciation of elemental/organic carbon). The main source contribution to BC concentrations in the urban site is traffic, accounting for 71.1%/65.2% (January/July) in close agreement with the fossil contribution derived from observations (78.8%/84.2%), followed by RWC (12.8%/3%) and shipping emissions (5.4%/13.8%). An over-representation of RWC (winter) and shipping (summer) is obtained with CAMS-REG_v4. Noteworthy uncertainties arise in OA results due to condensables in emissions and a limited secondary aerosol production in the model.These findings offer insights into MONARCH’s effectiveness in simulating CAs concentrations and source contribution in Northeast Spain. The study highlights the benefits of combining new datasets and modeling techniques to refine emission inventories and better understand and mitigate air pollution impacts.