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New particle formation (NPF) is a major source of aerosol particles and cloud condensation nuclei in the troposphere, playing an important role in both air quality and climate. Frequent NPF events have been observed in heavily polluted urban environments, contributing to the aerosol number concentration by a significant amount. The Po Valley region in northern Italy has been characterized as a hotspot for high aerosol loadings and frequent NPF events in southern Europe. However, the mechanisms of NPF and growth in this region are not completely understood. In this study, we conducted a continuous 2-month measurement campaign with state-of-the-art instruments to elucidate the NPF and growth mechanisms in northern Italy. Our results demonstrate that frequent NPF events (66 % of all days during the measurement campaign) are primarily driven by abundant sulfuric acid (8.5×106 cm−3) and basic molecules in this area. In contrast, oxygenated organic molecules from the atmospheric oxidation of volatile organic compounds (VOCs) appear to play a minor role in the initial cluster formation but contribute significantly to the consecutive growth process. Regarding alkaline molecules, amines are insufficient to stabilize all sulfuric acid clusters in the Po Valley. Ion cluster measurements and kinetic models suggest that ammonia (10 ppb) must therefore also play a role in the nucleation process. Generally, the high formation rates of sub-2 nm particles (87 cm−3 s−1) and nucleation-mode growth rates (5.1 nm h−1) as well as the relatively low condensational sink (8.9×10-3 s−1) will result in a high survival probability for newly formed particles, making NPF crucial for the springtime aerosol number budget. Our results also indicate that reducing key pollutants, such as SO2, amine and NH3, could help to substantially decrease the particle number concentrations in the Po Valley region.

We present an evaluation of the regional chemical transport model (CTM) WRF-CHIMERE (v2020r2) for the formation of biogenic secondary organic aerosol (BSOA) with a focus over the Finnish boreal forest. Formation processes of biogenic aerosols are still affected by different sources of uncertainties, and model predictions vary greatly depending on the levels of details of the adopted chemical and emissions schemes. In this study, air quality simulations were conducted for the summer of 2019 using different organic aerosol (OA) schemes (as currently available in the literature) to treat the formation of BSOA. First, we performed a set of simulations in the framework of the volatility basis set (VBS) scheme carrying different assumptions for the treatment of the aging processes of BSOA. The results of the model were compared against high-resolution (i.e., 1 h) organic aerosol mass and size distribution measurements performed at the Station for Measuring Ecosystem–Atmosphere Relations (SMEAR-II) site located in Hyytiälä, in addition to other gas-phase species such as ozone (O3), nitrogen oxides (NOx), and biogenic volatile organic compound (BVOC) measurements of isoprene (C5H10) and monoterpenes. We show that WRF-CHIMERE could reproduce well the diurnal variation of the measured OA concentrations for all the investigated scenarios (along with the standard meteorological parameters) as well as the increase in concentrations during specific heat wave episodes. However, the modeled OA concentrations varied greatly between the schemes used to describe the aging processes of BSOA, as also confirmed by an additional evaluation using organic carbon (OC) measurement data retrieved from the EBAS European databases. Comparisons with isoprene and monoterpene air concentrations revealed that the model captured the observed monoterpene concentrations, but isoprene was largely overestimated, a feature that was mainly attributed to the overstated biogenic emissions of isoprene. We investigated the potential consequences of such an overestimation by inhibiting isoprene emissions from the modeling system. Results indicated that the modeled BSOA concentrations increased in the northern regions of the domain (e.g., Finland) compared to southern European countries, possibly due to a shift in the reactions of monoterpene compounds against available radicals, as further suggested by the reduction in α-pinene modeled air concentrations. Finally, we briefly analyze the differences in the modeled cloud liquid water content (clwc) among the simulations carrying different chemical schemes for the treatment of the aging processes of BSOA. The results of the model indicated an increase in clwc values at the SMEAR-II site, for simulations with higher biogenic organic aerosol loads, most likely as a result of the increased number of biogenic aerosol particles capable of activating cloud droplets.

The Eurodelta-Trends (EDT) multi-model experiment, aimed at assessing the efficiency of emission mitigation measures in improving air quality in Europe during 1990–2010, was designed to answer a series of questions regarding European pollution trends; i.e. were there significant trends detected by observations? Do the models manage to reproduce observed trends? How close is the agreement between the models and how large are the deviations from observations? In this paper, we address these issues with respect to particulate matter (PM) pollution. An in-depth trend analysis has been performed for PM10 and PM2.5 for the period of 2000–2010, based on results from six chemical transport models and observational data from the EMEP (Cooperative Programme for Monitoring and Evaluation of the Long-range Transmission of Air Pollutants in Europe) monitoring network. Given harmonization of set-up and main input data, the differences in model results should mainly result from differences in the process formulations within the models themselves, and the spread in the model-simulated trends could be regarded as an indicator for modelling uncertainty. The model ensemble simulations indicate overall decreasing trends in PM10 and PM2.5 from 2000 to 2010, with the total reductions of annual mean concentrations by between 2 and 5 (7 for PM10) µg m−3 (or between 10 % and 30 %) across most of Europe (by 0.5–2 µg m−3 in Fennoscandia, the north-west of Russia and eastern Europe) during the studied period. Compared to PM2.5, relative PM10 trends are weaker due to large inter-annual variability of natural coarse PM within the former. The changes in the concentrations of PM individual components are in general consistent with emission reductions. There is reasonable agreement in PM trends estimated by the individual models, with the inter-model variability below 30 %–40 % over most of Europe, increasing to 50 %–60 % in the northern and eastern parts of the EDT domain. Averaged over measurement sites (26 for PM10 and 13 for PM2.5), the mean ensemble-simulated trends are −0.24 and −0.22 µg m−3 yr−1 for PM10 and PM2.5, which are somewhat weaker than the observed trends of −0.35 and −0.40 µg m−3 yr−1 respectively, partly due to model underestimation of PM concentrations. The correspondence is better in relative PM10 and PM2.5 trends, which are −1.7 % yr−1 and −2.0 % yr−1 from the model ensemble and −2.1 % yr−1 and −2.9 % yr−1 from the observations respectively. The observations identify significant trends (at the 95 % confidence level) for PM10 at 56 % of the sites and for PM2.5 at 36 % of the sites, which is somewhat less that the fractions of significant modelled trends. Further, we find somewhat smaller spatial variability of modelled PM trends with respect to the observed ones across Europe and also within individual countries. The strongest decreasing PM trends and the largest number of sites with significant trends are found for the summer season, according to both the model ensemble and observations. The winter PM trends are very weak and mostly insignificant. Important reasons for that are the very modest reductions and even increases in the emissions of primary PM from residential heating in winter. It should be kept in mind that all findings regarding modelled versus observed PM trends are limited to the regions where the sites are located. The analysis reveals considerable variability of the role of the individual aerosols in PM10 trends across European countries. The multi-model simulations, supported by available observations, point to decreases in SO4-2 concentrations playing an overall dominant role. Also, we see relatively large contributions of the trends of NH4+ and NO3- to PM10 decreasing trends in Germany, Denmark, Poland and the Po Valley, while the reductions of primary PM emissions appear to be a dominant factor in bringing down PM10 in France, Norway, Portugal, Greece and parts of the UK and Russia. Further discussions are given with respect to emission uncertainties (including the implications of not accounting for forest fires and natural mineral dust by some of the models) and the effect of inter-annual meteorological variability on the trend analysis.

A source-resolved three-dimensional chemical transport model, PMCAMx-SR (Particulate Matter Comprehensive Air-quality Model with extensions – Source Resolved), was applied in the continental US to investigate the contribution of the various components (primary and secondary) of biomass burning organic aerosol (bbOA) to organic aerosol levels. Two different schemes based on the volatility basis set were used for the simulation of the bbOA during different seasons. The first is the default scheme of PMCAMx-SR, and the second is a recently developed scheme based on laboratory experiments of the bbOA evolution. The simulations with the alternative bbOA scheme predict much higher total bbOA concentrations when compared with the base case ones. This is mainly due to the high emissions of intermediate-volatility organic compounds (IVOCs) assumed in the alternative scheme. The oxidation of these compounds is predicted to be a significant source of secondary organic aerosol. The impact of the other parameters that differ in the two schemes is low to negligible. The monthly average maximum predicted concentrations of the alternative bbOA scheme were approximately an order of magnitude higher than those of the default scheme during all seasons. The performance of the two schemes was evaluated against observed total organic aerosol concentrations from several measurement sites across the US. The results were different for the different seasons examined. The default scheme performed better during July and September, while the alternative scheme performed a little better during April. These results illustrate the uncertainty of the corresponding predictions and the need to quantify the emissions and reactions of IVOCs from specific biomass sources and to better constrain the total (primary and secondary) bbOA levels.

The focus of this modeling study is on the role of ammonia in European air quality in the past as well as in the future. Ammonia emissions have not decreased as much as the other secondary inorganic aerosol (SIA) precursors – nitrogen oxides (NOx) and sulfur dioxide (SO2) – since the 1990s and are still posing problems for air quality and the environment. In this study, air quality simulations were performed with a regional chemical transport model at decadal intervals between 1990 and 2030 to understand the changes in the chemical species associated with SIA under varying land and ship emissions. We analyzed the changes in air concentrations of ammonia, nitric acid, ammonium, particulate nitrate and sulfate as well as changes in the dry and wet deposition of ammonia and ammonium. The results show that the approximately 40 % decrease in SIA concentrations between 1990 and 2010 was mainly due to reductions in NOx and SO2 emissions. The ammonia concentrations on the other hand decreased only near the high-emission areas such as the Netherlands and northern Italy by about 30 %, while there was a slight increase in other parts of Europe. Larger changes in concentrations occurred mostly during the first period (1990–2000). The model results indicate a transition period after 2000 for the composition of secondary inorganic aerosols due to a larger decrease in sulfate concentrations than nitrate. Changes between 2010 and 2030 – assuming the current legislation (CLE) scenario – are predicted to be smaller than those achieved earlier for all species analyzed in this study. The scenario simulations suggest that if ship emissions will be regulated more strictly in the future, SIA formation will decrease especially around the Benelux area, North Sea, Baltic Sea, English Channel and the Mediterranean region, leaving more ammonia in the gas phase, which would lead to an increase in dry deposition. In the north of the domain, the decrease in SIA would be mainly due to reduced formation of particulate nitrate, while the change around the Mediterranean would be caused mainly by decreased sulfate aerosol concentrations. One should also keep in mind that potentially higher temperatures in the future might increase the evaporation of ammonium nitrate to form its gaseous components NH3 and HNO3. Sensitivity tests with reduced NOx and NH3 emissions indicate a shift in the sensitivity of aerosol formation from NH3 towards NOx emissions between 1990 and 2030 in most of Europe except the eastern part of the model domain.

Source apportionment of organic aerosols (OAs) is of great importance to better understand the health impact and climate effects of particulate matter air pollution. Air quality models are used as potential tools to identify OA components and sources at high spatial and temporal resolution; however, they generally underestimate OA concentrations, and comparisons of their outputs with an extended set of measurements are still rare due to the lack of long-term experimental data. In this study, we addressed such challenges at the European level. Using the regional Comprehensive Air Quality Model with Extensions (CAMx) and a volatility basis set (VBS) scheme which was optimized based on recent chamber experiments with wood burning and diesel vehicle emissions, and which contains more source-specific sets compared to previous studies, we calculated the contribution of OA components and defined their sources over a whole-year period (2011). We modeled separately the primary and secondary OA contributions from old and new diesel and gasoline vehicles, biomass burning (mostly residential wood burning and agricultural waste burning excluding wildfires), other anthropogenic sources (mainly shipping, industry and energy production) and biogenic sources. An important feature of this study is that we evaluated the model results with measurements over a longer period than in previous studies, which strengthens our confidence in our modeled source apportionment results. Comparison against positive matrix factorization (PMF) analyses of aerosol mass spectrometric measurements at nine European sites suggested that the modified VBS scheme improved the model performance for total OA as well as the OA components, including hydrocarbon-like (HOA), biomass burning (BBOA) and oxygenated components (OOA). By using the modified VBS scheme, the mean bias of OOA was reduced from −1.3 to −0.4 µg m−3 corresponding to a reduction of mean fractional bias from −45 % to −20 %. The winter OOA simulation, which was largely underestimated in previous studies, was improved by 29 % to 42 % among the evaluated sites compared to the default parameterization. Wood burning was the dominant OA source in winter (61 %), while biogenic emissions contributed ∼ 55 % to OA during summer in Europe on average. In both seasons, other anthropogenic sources comprised the second largest component (9 % in winter and 19 % in summer as domain average), while the average contributions of diesel and gasoline vehicles were rather small (∼ 5 %) except for the metropolitan areas where the highest contribution reached 31 %. The results indicate the need to improve the emission inventory to include currently missing and highly uncertain local emissions, as well as further improvement of VBS parameterization for winter biomass burning. Although this study focused on Europe, it can be applied in any other part of the globe. This study highlights the ability of long-term measurements and source apportionment modeling to validate and improve emission inventories, and identify sources not yet properly included in existing inventories.

In the framework of the EURODELTA-Trends (EDT) modeling experiment, several chemical transport models (CTMs) were applied for the 1990–2010 period to investigate air quality changes in Europe as well as the capability of the models to reproduce observed long-term air quality trends. Five CTMs have provided modeled air quality data for 21 continuous years in Europe using emission scenarios prepared by the International Institute for Applied Systems Analysis/Greenhouse Gas – Air Pollution Interactions and Synergies (IIASA/GAINS) and corresponding year-by-year meteorology derived from ERA-Interim global reanalysis. For this study, long-term observations of particle sulfate (SO42-), total nitrate (TNO3), total ammonium (TNHx) as well as sulfur dioxide (SO2) and nitrogen dioxide (NO2) for multiple sites in Europe were used to evaluate the model results. The trend analysis was performed for the full 21 years (referred to as PT) but also for two 11-year subperiods: 1990–2000 (referred to as P1) and 2000–2010 (referred to as P2). The experiment revealed that the models were able to reproduce the faster decline in observed SO2 concentrations during the first decade, i.e., 1990–2000, with a 64 %–76 % mean relative reduction in SO2 concentrations indicated by the EDT experiment (range of all the models) versus an 82 % mean relative reduction in observed concentrations. During the second decade (P2), the models estimated a mean relative reduction in SO2 concentrations of about 34 %–54 %, which was also in line with that observed (47 %). Comparisons of observed and modeled NO2 trends revealed a mean relative decrease of 25 % and between 19 % and 23 % (range of all the models) during the P1 period, and 12 % and between 22 % and 26 % (range of all the models) during the P2 period, respectively. Comparisons of observed and modeled trends in SO42- concentrations during the P1 period indicated that the models were able to reproduce the observed trends at most of the sites, with a 42 %–54 % mean relative reduction indicated by the EDT experiment (range of all models) versus a 57 % mean relative reduction in observed concentrations and with good performance also during the P2 and PT periods, even though all the models overpredicted the number of statistically significant decreasing trends during the P2 period. Moreover, especially during the P1 period, both modeled and observational data indicated smaller reductions in SO42- concentrations compared with their gas-phase precursor (i.e., SO2), which could be mainly attributed to increased oxidant levels and pH-dependent cloud chemistry. An analysis of the trends in TNO3 concentrations indicated a 28 %–39 % and 29 % mean relative reduction in TNO3 concentrations for the full period for model data (range of all the models) and observations, respectively. Further analysis of the trends in modeled HNO3 and particle nitrate (NO3-) concentrations revealed that the relative reduction in HNO3 was larger than that for NO3- during the P1 period, which was mainly attributed to an increased availability of “free ammonia”. By contrast, trends in modeled HNO3 and NO3- concentrations were more comparable during the P2 period. Also, trends of TNHx concentrations were, in general, underpredicted by all models, with worse performance for the P1 period than for P2. Trends in modeled anthropogenic and biogenic secondary organic aerosol (ASOA and BSOA) concentrations together with the trends in available emissions of biogenic volatile organic compounds (BVOCs) were also investigated. A strong decrease in ASOA was indicated by all the models, following the reduction in anthropogenic non-methane VOC (NMVOC) precursors. Biogenic emission data provided by the modeling teams indicated a few areas with statistically significant increase in isoprene emissions and monoterpene emissions during the 1990–2010 period over Fennoscandia and eastern European regions (i.e., around 14 %–27 %), which was mainly attributed to the increase of surface temperature. However, the modeled BSOA concentrations did not linearly follow the increase in biogenic emissions. Finally, a comprehensive evaluation against positive matrix factorization (PMF) data, available during the second period (P2) at various European sites, revealed a systematic underestimation of the modeled SOA fractions of a factor of 3 to 11, on average, most likely because of missing SOA precursors and formation pathways, with reduced biases for the models that accounted for chemical aging of semi-volatile SOA components in the atmosphere.

Organic aerosol (OA) can have important impacts on air quality and human health because of its large contribution to atmospheric fine aerosol and its chemical composition, including many toxic compounds. Simulation of this type of aerosol is difficult, since there are many unknowns in its nature and mechanism and processes involved in its formation. These uncertainties become even more important in the context of a changing climate because different mechanisms, and their representation in atmospheric models, imply different sensitivities to changes in climate variables. In this work, the effects caused by using different schemes to simulate OA are explored. Three schemes are used in this work: (1) a molecular scheme; (2) a standard volatility basis set (VBS) scheme with anthropogenic aging; and (3) a modified VBS scheme containing functionalization, fragmentation and formation of nonvolatile secondary organic aerosol (SOA) for all semi-volatile organic compounds (SVOCs). Five years of historic and five years of future simulations were performed using the RCP8.5 climatic scenario. The years were chosen in a way to maximize the differences between future and historic simulations. The study focuses on biogenic SOA (BSOA), since the contribution of this fraction of BSOA among OA is major in both historic and future scenarios (40 % to 78 % for different schemes in historic simulations). Simulated OA and BSOA concentrations with different schemes are different, with the molecular scheme showing the highest concentrations among the three schemes. The comparisons show that for the European area, the modified VBS scheme shows the highest relative change between future and historic simulations, while the molecular scheme shows the lowest (a factor of 2 lower). These changes are largest over the summer period for BSOA because the higher temperatures increase terpene and isoprene emissions, the major precursors of BSOA. This increase is partially offset by a temperature-induced shift of SVOCs to the gas phase. This shift is indeed scheme dependent, and it is shown that it is the least pronounced for the modified VBS scheme including a full suite of aerosol aging processes, comprising also formation of nonvolatile aerosol. For the Mediterranean Sea, without BVOC emissions, the OA changes are less pronounced and, at least on an annual average, more similar between different schemes. Our results warrant further developments in organic aerosol schemes used for air quality modeling to reduce their uncertainty, including sensitivity to climate variables (temperature).

Multiple CMIP5 (Coupled Model Intercomparison Project phase 5) future scenarios run with the CHIMERE chemistry transport model (CTM) are compared to historic simulations in order to study some of the drivers governing air pollution. Here, the focus is on regional climate, anthropogenic emissions and long-range transport. Two major subdomains are explored – the European region and the Mediterranean Basin – with both areas showing high sensitivity to climate change. The Mediterranean area is explored in the context of the ChArMEx (the Chemistry Aerosol Mediterranean Experiment) project, which examines the current and future meteorological and chemical conditions of the Mediterranean area. This climate impact study covers the period from 2031 to 2100 and considers possible future scenarios in comparison with 1976 to 2005 historic simulations using three Representative Concentration Pathways (RCPs; RCP2.6, RCP4.5 and RCP8.5). A detailed analysis of total PM10 (particulate matter with a diameter smaller that 10 µm) concentrations is carried out, including the evolution of PM10 and changes to its composition. The individual effects of meteorological conditions on PM10 components are explored in these scenarios in an effort to pinpoint the meteorological parameter(s) governing each component. The anthropogenic emission impact study covers the period from 2046 to 2055 using current legislation (CLE) and maximum feasible reduction (MFR) anthropogenic emissions for the year 2050 compared with historic simulations covering the period from 1996 to 2005 and utilizing CLE2010 emissions data. Long-range transport is explored by changing the boundary conditions in the chemistry transport model over the same period as the emission impact studies. Finally, a cumulative effect analysis of these drivers is performed, and the impact of each driver on PM10 and its components is estimated. The results show that regional climate change causes a decrease in the PM10 concentrations in our scenarios (in both the European and Mediterranean subdomains), as a result of a decrease in nitrate, sulfate, ammonium and dust atmospheric concentrations in most scenarios. On the contrary, BSOA (biogenic secondary organic aerosol) displays an important increase in all scenarios, showing more pronounced concentrations for the European subdomain compared with the Mediterranean region. Regarding the relationship of different meteorological parameters to concentrations of different species, nitrate and BSOA show a strong temperature dependence, whereas sulfate is most strongly correlated with relative humidity. The temperature-dependent behavior of BSOA changes when looking at the Mediterranean subdomain, where it displays more dependence on wind speed, due to the transported nature of BSOA existing in this subdomain. A cumulative look at all drivers shows that anthropogenic emission changes overshadow changes caused by climate and long-range transport for both of the subdomains explored, with the exception of dust particles for which long-range transport changes are more influential, especially in the Mediterranean Basin. For certain species (such as sulfates and BSOA), in most of the subdomains explored, the changes caused by anthropogenic emissions are (to a certain extent) reduced by the boundary conditions and regional climate changes.

Biogenic volatile organic compound (BVOC) emissions are one of the essential inputs for chemical transport models (CTMs), but their estimates are associated with large uncertainties, leading to significant influence on air quality modelling. This study aims to investigate the effects of using different BVOC emission models on the performance of a CTM in simulating secondary pollutants, i.e. ozone, organic, and inorganic aerosols. European air quality was simulated for the year 2011 by the regional air quality model Comprehensive Air Quality Model with Extensions (CAMx) version 6.3, using BVOC emissions calculated by two emission models: the Paul Scherrer Institute (PSI) model and the Model of Emissions of Gases and Aerosol from Nature (MEGAN) version 2.1. Comparison of isoprene and monoterpene emissions from both models showed large differences in their general amounts, as well as their spatial distribution in both summer and winter. MEGAN produced more isoprene emissions by a factor of 3 while the PSI model generated 3 times the monoterpene emissions in summer, while there was negligible difference (∼4 %) in sesquiterpene emissions associated with the two models. Despite the large differences in isoprene emissions (i.e. 3-fold), the resulting impact in predicted summertime ozone proved to be minor (<10 %; MEGAN O3 was higher than PSI O3 by ∼7 ppb). Comparisons with measurements from the European air quality database (AirBase) indicated that PSI emissions might improve the model performance at low ozone concentrations but worsen performance at high ozone levels (>60 ppb). A much larger effect of the different BVOC emissions was found for the secondary organic aerosol (SOA) concentrations. The higher monoterpene emissions (a factor of ∼3) by the PSI model led to higher SOA by ∼110 % on average in summer, compared to MEGAN, and lead to better agreement between modelled and measured organic aerosol (OA): the mean bias between modelled and measured OA at nine measurement stations using Aerodyne aerosol chemical speciation monitors (ACSMs) or Aerodyne aerosol mass spectrometers (AMSs) was reduced by 21 %–83 % at rural or remote stations. Effects on inorganic aerosols (particulate nitrate, sulfate, and ammonia) were relatively small (<15 %).

The wet deposition of nitrogen and sulfur in Europe for the period 1990–2010 was estimated by six atmospheric chemistry transport models (CHIMERE, CMAQ, EMEP MSC-W, LOTOS-EUROS, MATCH and MINNI) within the framework of the EURODELTA-Trends model intercomparison. The simulated wet deposition and its trends for two 11-year periods (1990–2000 and 2000–2010) were evaluated using data from observations from the EMEP European monitoring network. For annual wet deposition of oxidised nitrogen (WNOx), model bias was within 30 % of the average of the observations for most models. There was a tendency for most models to underestimate annual wet deposition of reduced nitrogen (WNHx), although the model bias was within 40 % of the average of the observations. Model bias for WNHx was inversely correlated with model bias for atmospheric concentrations of NH3+NH4+, suggesting that an underestimation of wet deposition partially contributed to an overestimation of atmospheric concentrations. Model bias was also within about 40 % of the average of the observations for the annual wet deposition of sulfur (WSOx) for most models. Decreasing trends in WNOx were observed at most sites for both 11-year periods, with larger trends, on average, for the second period. The models also estimated predominantly decreasing trends at the monitoring sites and all but one of the models estimated larger trends, on average, for the second period. Decreasing trends were also observed at most sites for WNHx, although larger trends, on average, were observed for the first period. This pattern was not reproduced by the models, which estimated smaller decreasing trends, on average, than those observed or even small increasing trends. The largest observed trends were for WSOx, with decreasing trends at more than 80 % of the sites. On average, the observed trends were larger for the first period. All models were able to reproduce this pattern, although some models underestimated the trends (by up to a factor of 4) and others overestimated them (by up to 40 %), on average. These biases in modelled trends were directly related to the tendency of the models to under- or overestimate annual wet deposition and were smaller for the relative trends (expressed as % yr−1 relative to the deposition at the start of the period). The fact that model biases were fairly constant throughout the time series makes it possible to improve the predictions of wet deposition for future scenarios by adjusting the model estimates using a bias correction calculated from past observations. An analysis of the contributions of various factors to the modelled trends suggests that the predominantly decreasing trends in wet deposition are mostly due to reductions in emissions of the precursors NOx, NH3 and SOx. However, changes in meteorology (e.g. precipitation) and other (non-linear) interactions partially offset the decreasing trends due to emission reductions during the first period but not the second. This suggests that the emission reduction measures had a relatively larger effect on wet deposition during the second period, at least for the sites with observations.

Surface solar radiation (SSR) observations have indicated an increasing trend in Europe since the mid-1980s, referred to as solar brightening. In this study, we used the regional air quality model, CAMx (Comprehensive Air Quality Model with Extensions) to simulate and quantify, with various sensitivity runs (where the year 2010 served as the base case), the effects of increased radiation between 1990 and 2010 on photolysis rates (with the PHOT1, PHOT2 and PHOT3 scenarios, which represented the radiation in 1990) and biogenic volatile organic compound (BVOC) emissions (with the BIO scenario, which represented the biogenic emissions in 1990), and their consequent impacts on summer surface ozone concentrations over Europe between 1990 and 2010. The PHOT1 and PHOT2 scenarios examined the effect of doubling and tripling the anthropogenic PM2.5 concentrations, respectively, while the PHOT3 investigated the impact of an increase in just the sulfate concentrations by a factor of 3.4 (as in 1990), applied only to the calculation of photolysis rates. In the BIO scenario, we reduced the 2010 SSR by 3 % (keeping plant cover and temperature the same), recalculated the biogenic emissions and repeated the base case simulations with the new biogenic emissions. The impact on photolysis rates for all three scenarios was an increase (in 2010 compared to 1990) of 3–6 % which resulted in daytime (10:00–18:00 Local Mean Time – LMT) mean surface ozone differences of 0.2–0.7 ppb (0.5–1.5 %), with the largest hourly difference rising as high as 4–8 ppb (10–16 %). The effect of changes in BVOC emissions on daytime mean surface ozone was much smaller (up to 0.08 ppb, ∼ 0.2 %), as isoprene and terpene (monoterpene and sesquiterpene) emissions increased only by 2.5–3 and 0.7 %, respectively. Overall, the impact of the SSR changes on surface ozone was greater via the effects on photolysis rates compared to the effects on BVOC emissions, and the sensitivity test of their combined impact (the combination of PHOT3 and BIO is denoted as the COMBO scenario) showed nearly additive effects. In addition, all the sensitivity runs were repeated on a second base case with increased NOx emissions to account for any potential underestimation of modeled ozone production; the results did not change significantly in magnitude, but the spatial coverage of the effects was profoundly extended. Finally, the role of the aerosol–radiation interaction (ARI) changes in the European summer surface ozone trends was suggested to be more important when comparing to the order of magnitude of the ozone trends instead of the total ozone concentrations, indicating a potential partial damping of the effects of ozone precursor emissions' reduction.

High surface ozone concentrations, which usually occur when photochemical ozone production takes place, pose a great risk to human health and vegetation. Air quality models are often used by policy makers as tools for the development of ozone mitigation strategies. However, the modeled ozone production is often not or not enough evaluated in many ozone modeling studies. The focus of this work is to evaluate the modeled ozone production in Europe indirectly, with the use of the ozone–temperature correlation for the summer of 2010 and to analyze its sensitivity to precursor emissions and meteorology by using the regional air quality model, the Comprehensive Air Quality Model with Extensions (CAMx). The results show that the model significantly underestimates the observed high afternoon surface ozone mixing ratios (≥ 60 ppb) by 10–20 ppb and overestimates the lower ones (x) emissions by a factor of 2, (iii) a combination of the first two scenarios and (iv) increased traffic-only NOx emissions by a factor of 4. For southern, eastern, and central (except the Benelux area) Europe, doubling NOx emissions seems to be the most efficient scenario to reduce the underestimation of the observed high ozone mixing ratios without significant degradation of the model performance for the lower ozone mixing ratios. The model performance for ozone–temperature correlation is also better when NOx emissions are doubled. In the Benelux area, however, the third scenario (where both NOx and VOC emissions are increased) leads to a better model performance. Although increasing only the traffic NOx emissions by a factor of 4 gave very similar results to the doubling of all NOx emissions, the first scenario is more consistent with the uncertainties reported by other studies than the latter, suggesting that high uncertainties in NOx emissions might originate mainly from the road-transport sector rather than from other sectors. The impact of meteorology was examined with three sensitivity tests: (i) increased surface temperature by 4 °C, (ii) reduced wind speed by 50 % and (iii) doubled wind speed. The first two scenarios led to a consistent increase in all surface ozone mixing ratios, thus improving the model performance for the high ozone values but significantly degrading it for the low ozone values, while the third scenario had exactly the opposite effects. Overall, the modeled ozone is predicted to be more sensitive to its precursor emissions (especially traffic NOx) and therefore their uncertainties, which seem to be responsible for the model underestimation of the observed high ozone mixing ratios and ozone production.

We evaluated a modified VBS (volatility basis set) scheme to treat biomass-burning-like organic aerosol (BBOA) implemented in CAMx (Comprehensive Air Quality Model with extensions). The updated scheme was parameterized with novel wood combustion smog chamber experiments using a hybrid VBS framework which accounts for a mixture of wood burning organic aerosol precursors and their further functionalization and fragmentation in the atmosphere. The new scheme was evaluated for one of the winter EMEP intensive campaigns (February–March 2009) against aerosol mass spectrometer (AMS) measurements performed at 11 sites in Europe. We found a considerable improvement for the modelled organic aerosol (OA) mass compared to our previous model application with the mean fractional bias (MFB) reduced from −61 to −29 %. We performed model-based source apportionment studies and compared results against positive matrix factorization (PMF) analysis performed on OA AMS data. Both model and observations suggest that OA was mainly of secondary origin at almost all sites. Modelled secondary organic aerosol (SOA) contributions to total OA varied from 32 to 88 % (with an average contribution of 62 %) and absolute concentrations were generally under-predicted. Modelled primary hydrocarbon-like organic aerosol (HOA) and primary biomass-burning-like aerosol (BBPOA) fractions contributed to a lesser extent (HOA from 3 to 30 %, and BBPOA from 1 to 39 %) with average contributions of 13 and 25 %, respectively. Modelled BBPOA fractions were found to represent 12 to 64 % of the total residential-heating-related OA, with increasing contributions at stations located in the northern part of the domain. Source apportionment studies were performed to assess the contribution of residential and non-residential combustion precursors to the total SOA. Non-residential combustion and road transportation sector contributed about 30–40 % to SOA formation (with increasing contributions at urban and near industrialized sites), whereas residential combustion (mainly related to wood burning) contributed to a larger extent, around 60–70 %. Contributions to OA from residential combustion precursors in different volatility ranges were also assessed: our results indicate that residential combustion gas-phase precursors in the semivolatile range (SVOC) contributed from 6 to 30 %, with higher contributions predicted at stations located in the southern part of the domain. On the other hand, the oxidation products of higher-volatility precursors (the sum of intermediate-volatility compounds (IVOCs) and volatile organic compounds (VOCs)) contribute from 15 to 38 % with no specific gradient among the stations. Although the new parameterization leads to a better agreement between model results and observations, it still under-predicts the SOA fraction, suggesting that uncertainties in the new scheme and other sources and/or formation mechanisms remain to be elucidated. Moreover, a more detailed characterization of the semivolatile components of the emissions is needed.

Contributions of various anthropogenic sources to the secondary inorganic aerosol (SIA) in Europe as well as the role of biogenic emissions on SIA formation were investigated using the three-dimensional regional model CAMx (comprehensive air quality model with extensions). Simulations were carried out for two periods of EMEP field campaigns, February–March 2009 and June 2006, which are representative of cold and warm seasons, respectively. Biogenic volatile organic compounds (BVOCs) are known mainly as precursors of ozone and secondary organic aerosol (SOA), but their role on inorganic aerosol formation has not attracted much attention so far. In this study, we showed the importance of the chemical reactions of BVOCs and how they affect the oxidant concentrations, leading to significant changes, especially in the formation of ammonium nitrate. A sensitivity test with doubled BVOC emissions in Europe during the warm season showed a large increase in secondary organic aerosol (SOA) concentrations (by about a factor of two), while particulate inorganic nitrate concentrations decreased by up to 35 %, leading to a better agreement between the model results and measurements. Sulfate concentrations decreased as well; the change, however, was smaller. The changes in inorganic nitrate and sulfate concentrations occurred at different locations in Europe, indicating the importance of precursor gases and biogenic emission types for the negative correlation between BVOCs and SIA. Further analysis of the data suggested that reactions of the additional terpenes with nitrate radicals at night were responsible for the decline in inorganic nitrate formation, whereas oxidation of BVOCs with OH radicals led to a decrease in sulfate. Source apportionment results suggest that the main anthropogenic source of precursors leading to formation of particulate inorganic nitrate is road transport (SNAP7; see Table 1 for a description of the categories), whereas combustion in energy and transformation industries (SNAP1) was the most important contributor to sulfate particulate mass. Emissions from international shipping were also found to be very important for both nitrate and sulfate formation in Europe. In addition, we also examined contributions from the geographical source regions to SIA concentrations in the most densely populated region of Switzerland, the Swiss Plateau.

In this study, novel wood combustion aging experiments performed at different temperatures (263 and 288 K) in a ∼ 7 m3 smog chamber were modelled using a hybrid volatility basis set (VBS) box model, representing the emission partitioning and their oxidation against OH. We combine aerosol–chemistry box-model simulations with unprecedented measurements of non-traditional volatile organic compounds (NTVOCs) from a high-resolution proton transfer reaction mass spectrometer (PTR-MS) and with organic aerosol measurements from an aerosol mass spectrometer (AMS). Due to this, we are able to observationally constrain the amounts of different NTVOC aerosol precursors (in the model) relative to low volatility and semi-volatile primary organic material (OMsv), which is partitioned based on current published volatility distribution data. By comparing the NTVOC ∕ OMsv ratios at different temperatures, we determine the enthalpies of vaporization of primary biomass-burning organic aerosols. Further, the developed model allows for evaluating the evolution of oxidation products of the semi-volatile and volatile precursors with aging. More than 30 000 box-model simulations were performed to retrieve the combination of parameters that best fit the observed organic aerosol mass and O : C ratios. The parameters investigated include the NTVOC reaction rates and yields as well as enthalpies of vaporization and the O : C of secondary organic aerosol surrogates. Our results suggest an average ratio of NTVOCs to the sum of non-volatile and semi-volatile organic compounds of ∼ 4.75. The mass yields of these compounds determined for a wide range of atmospherically relevant temperatures and organic aerosol (OA) concentrations were predicted to vary between 8 and 30 % after 5 h of continuous aging. Based on the reaction scheme used, reaction rates of the NTVOC mixture range from 3.0 × 10−11 to 4. 0 × 10−11 cm3 molec−1 s−1. The average enthalpy of vaporization of secondary organic aerosol (SOA) surrogates was determined to be between 55 000 and 35 000 J mol−1, which implies a yield increase of 0.03–0.06 % K−1 with decreasing temperature. The improved VBS scheme is suitable for implementation into chemical transport models to predict the burden and oxidation state of primary and secondary biomass-burning aerosols.

The EURODELTA III exercise has facilitated a comprehensive intercomparison and evaluation of chemistry transport model performances. Participating models performed calculations for four 1-month periods in different seasons in the years 2006 to 2009, allowing the influence of different meteorological conditions on model performances to be evaluated. The exercise was performed with strict requirements for the input data, with few exceptions. As a consequence, most of differences in the outputs will be attributed to the differences in model formulations of chemical and physical processes. The models were evaluated mainly for background rural stations in Europe. The performance was assessed in terms of bias, root mean square error and correlation with respect to the concentrations of air pollutants (NO2, O3, SO2, PM10 and PM2.5), as well as key meteorological variables. Though most of meteorological parameters were prescribed, some variables like the planetary boundary layer (PBL) height and the vertical diffusion coefficient were derived in the model preprocessors and can partly explain the spread in model results. In general, the daytime PBL height is underestimated by all models. The largest variability of predicted PBL is observed over the ocean and seas. For ozone, this study shows the importance of proper boundary conditions for accurate model calculations and then on the regime of the gas and particle chemistry. The models show similar and quite good performance for nitrogen dioxide, whereas they struggle to accurately reproduce measured sulfur dioxide concentrations (for which the agreement with observations is the poorest). In general, the models provide a close-to-observations map of particulate matter (PM2.5 and PM10) concentrations over Europe rather with correlations in the range 0.4–0.7 and a systematic underestimation reaching −10 µg m−3 for PM10. The highest concentrations are much more underestimated, particularly in wintertime. Further evaluation of the mean diurnal cycles of PM reveals a general model tendency to overestimate the effect of the PBL height rise on PM levels in the morning, while the intensity of afternoon chemistry leads formation of secondary species to be underestimated. This results in larger modelled PM diurnal variations than the observations for all seasons. The models tend to be too sensitive to the daily variation of the PBL. All in all, in most cases model performances are more influenced by the model setup than the season. The good representation of temporal evolution of wind speed is the most responsible for models' skillfulness in reproducing the daily variability of pollutant concentrations (e.g. the development of peak episodes), while the reconstruction of the PBL diurnal cycle seems to play a larger role in driving the corresponding pollutant diurnal cycle and hence determines the presence of systematic positive and negative biases detectable on daily basis.

Four periods of EMEP (European Monitoring and Evaluation Programme) intensive measurement campaigns (June 2006, January 2007, September–October 2008 and February–March 2009) were modelled using the regional air quality model CAMx with VBS (volatility basis set) approach for the first time in Europe within the framework of the EURODELTA-III model intercomparison exercise. More detailed analysis and sensitivity tests were performed for the period of February–March 2009 and June 2006 to investigate the uncertainties in emissions as well as to improve the modelling of organic aerosol (OA). Model performance for selected gas phase species and PM2.5 was evaluated using the European air quality database AirBase. Sulfur dioxide (SO2) and ozone (O3) were found to be overestimated for all the four periods, with O3 having the largest mean bias during June 2006 and January–February 2007 periods (8.9 pbb and 12.3 ppb mean biases respectively). In contrast, nitrogen dioxide (NO2) and carbon monoxide (CO) were found to be underestimated for all the four periods. CAMx reproduced both total concentrations and monthly variations of PM2.5 for all the four periods with average biases ranging from −2.1 to 1.0 µg m−3. Comparisons with AMS (aerosol mass spectrometer) measurements at different sites in Europe during February–March 2009 showed that in general the model overpredicts the inorganic aerosol fraction and underpredicts the organic one, such that the good agreement for PM2.5 is partly due to compensation of errors. The effect of the choice of VBS scheme on OA was investigated as well. Two sensitivity tests with volatility distributions based on previous chamber and ambient measurements data were performed. For February–March 2009 the chamber case reduced the total OA concentrations by about 42 % on average. In contrast, a test based on ambient measurement data increased OA concentrations by about 42 % for the same period bringing model and observations into better agreement. Comparison with the AMS data at the rural Swiss site Payerne in June 2006 shows no significant improvement in modelled OA concentration. Further sensitivity tests with increased biogenic and anthropogenic emissions suggest that OA in Payerne was affected by changes in emissions from residential heating during the February–March 2009 whereas it was more sensitive to biogenic precursors in June 2006.

We report a study of changes in air quality due to emission reductions using the chemical transport model CAMx. The model domain includes all of Europe with a nested domain over Switzerland. The model simulations were performed with emissions for 1990 (the reference year for the Gothenburg Protocol), 2005 (the reference year for the revised Gothenburg Protocol), 2006 (for model validation) and 2020 (the target year for the revised Gothenburg Protocol) using three emission scenarios prepared by IIASA/GAINS. Changes in ozone, particulate matter and nitrogen deposition are the central theme of the study. The modelled relative changes in the annual average PM2.5 concentrations between 1990 and 2005 look reasonable based on various PM10 and PM2.5 observations in the past. The results obtained in this study suggest that annual mean concentrations of PM2.5 decreased by about 20–50% in Europe. Simulations using the baseline scenario (BL 2020) suggest that PM2.5 concentrations in 2020 will be about 30% lower than those in 2005. The largest predicted decrease in PM2.5, based on the MTFR (maximum technically feasible reduction) scenario, was about 60% and was located mainly in the eastern part of Europe. In the case of ozone, both model results and measurements show an increase in the mean ozone mixing ratios between 1990 and 2005. The observations, however, suggest a larger increase, indicating the importance of background ozone levels. Although emission reductions caused a decrease in peak ozone values, average ozone levels in polluted regions increased due to reduced titration with nitric oxide (NO). This caused a change in the frequency distribution of ozone. Model simulations using emission scenarios for 2020 suggest that annual average ozone mixing ratios will continue to increase. Changes in the levels of the damage indicators AOT40 for forests and SOMO35 are reported as well. The model results suggest that nitrogen deposition has decreased by 10–30% in the eastern part of Europe since 1990, while it has increased by about 20% in the Iberian Peninsula. The decrease is mainly due to the deposition of oxidized nitrogen species, whereas deposition of reduced nitrogen compounds increased. In Switzerland, nitrogen deposition is larger in the northern part of the Alps, where ammonia emissions are the highest. Applying the baseline scenario, we found that the deposition of oxidized nitrogen compounds will have decreased by a further 40% by 2020, whereas deposition of reduced species will continue to increase. This will lead to a 10–20% decrease in the total nitrogen deposition in most of the model domain, with a 10% increase in the eastern part of Europe.

New particle formation (NPF) in the tropical free troposphere (FT) is a globally important source of cloud condensation nuclei, affecting cloud properties and climate. Oxidized organic molecules (OOMs) produced from biogenic volatile organic compounds are believed to contribute to aerosol formation in the tropical FT, but without direct chemical observations. We performed in situ molecular-level OOMs measurements at the Bolivian station Chacaltaya at 5240 m above sea level, on the western edge of Amazonia. For the first time, we demonstrate the presence of OOMs, mainly with 4-5 carbon atoms, in both gas-phase and particle-phase (in terms of mass contribution) measurements in tropical FT air from Amazonia. These observations, combined with air mass history analyses, indicate that the observed OOMs are linked to isoprene emitted from the rainforests hundreds of kilometers away. Based on particle-phase measurements, we find that these compounds can contribute to NPF, at least the growth of newly formed nanoparticles, in the tropical FT on a continental scale. Thus, our study is a fundamental and significant step in understanding the aerosol formation process in the tropical FT., (© The Author(s) 2023. Published by Oxford University Press on behalf of China Science Publishing & Media Ltd.)

The spread of COVID-19 has posed serious challenges for the global communities. To reduce the circulation of the infection, governmental bodies have imposed different lockdown measures at various levels of complexity and duration. As a result, a substantial reduction in mobility might have important, yet unknown, implications for air quality. In this study, we applied the Comprehensive Air quality Model with eXtensions (CAMx) to investigate potential changes in air quality and its chemical composition over northern Italy and Switzerland during periods when lockdown measures were enforced. Our results indicated that lockdown measures reduced nitrogen dioxide (NO 2 ) air concentrations by up to 46% and 25% in the Po Valley and Swiss Plateau regions, respectively, whereas fine particulate matter (PM 2.5 ) air concentrations were reduced only by up to 10% and 6%. This highlights the importance of other emission categories other than traffic for the total PM 2.5 levels. The analysis of the PM 2.5 components indicated that elemental carbon (EC) and particulate nitrate (NO 3 - ) were the species most affected by the lockdown measures, whereas a mild increase in the secondary organic aerosol (SOA) concentrations occurred in the Po Valley, and specifically over the metropolitan area of Milan. Our results indicated that an increase in the oxidation capacity of the atmosphere, i.e. in the ˙OH and ˙NO 3 radicals, was mainly responsible for the mild increase in SOA concentrations., Competing Interests: The authors declare no competing interests., (This journal is © The Royal Society of Chemistry.)

The lockdown measures implemented to curb the COVID-19 epidemic in Italy reduced human mobility dramatically, which resulted in a marked decline in traffic intensity. In this study, we present the effect of lockdown measures on several air pollutants, particle number size distribution as well as on regional new particle formation (NPF) frequency in the Po Valley (northern Italy). The results show that during the lockdown period, concentrations of nitrogen dioxide (NO 2 ), nitric oxide (NO), benzene (C 6 H 6 ), and toluene (C 7 H 8 ) decreased, while ozone (O 3 ) concentrations mildly increased as compared to the corresponding period in 2016-2019. Unlike gaseous pollutants, particulate matter mass concentrations (PM 2.5 and PM 10 ) showed no significant changes. The impact of lockdown measures on particle number size distributions were also quite limited. During the lockdown period, the number concentrations of 10-25 and 25-50 nm primary particles were reduced by 66% and 34%, respectively, at the regional background site (Ispra) but surprisingly there was no difference during and after lockdown at the urban background site (Modena). Conversely, the NPF frequency was exceptionally high, 70%, in Modena during the lockdown as compared to values (22-26%) observed for the same period in 2006 and 2009, while NPF frequency in Ispra only slightly increased compared to the same period in 2016-2019. The particle growth rates, however, were slightly lower during the lockdown at both sites compared to other periods. The study shows that a drastic decrease in traffic had little influence on particulate pollution levels in the Po Valley, suggesting that other sources and processes also have a prominent impact on particle number and particulate matter mass concentration in this region., Competing Interests: The authors declare no competing interests., (This journal is © The Royal Society of Chemistry.)

Air pollution is among the top threats to human health and ecosystems despite the substantial decrease in anthropogenic emissions. Meanwhile, the role of ship emissions on air quality is becoming increasingly important with the growing maritime transport and less strict regulations. In this study, we modeled the air quality in Europe between 1990 and 2030 with ten-year intervals, using the regional air quality model CAMx version 6.50, to investigate the changes in the past (1990-2010) as well as the effects of different land and ship emission scenarios in the future (2020,2030). The modeled mean ozone levels decreased slightly during the first decade but then started increasing again especially in polluted areas. Results from the future scenarios suggest that by 2030 the peak ozone would decrease, leading to a decrease in the days exceeding the maximum daily 8-h average ozone (MDA8) limit values (60 ppb) by 51% in southern Europe relative to 1990. The model results show a decrease of 56% (6.3 μg m -3 ) in PM 2.5 concentrations from 1990 to 2030 under current legislation, mostly due to a large drop in sulfate (representing up to 44% of the total PM 2.5 decrease during 1990-2000) while nitrate concentrations were predicted to go down with an increasing rate (10% of total PM 2.5 decrease during 1990-2000 while 36% during 2020-2030). The ship emissions if reduced according to the maximum technically feasible reduction (MTFR) scenario were predicted to contribute up to 19% of the decrease in the PM 2.5 concentrations over land between 2010 and 2030. Ship emission reductions according to the MTFR scenario would lead to a decrease in the days with MDA8 exceeding EU limits by 24-28% (10-14 days) around the coastal regions. The results obtained in our study show the increasing importance of ship emission reductions, after a relatively large decrease in land emissions was achieved in Europe., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2020 The Authors. Published by Elsevier B.V. All rights reserved.)

Rapid industrialization and urbanization in developing countries has led to an increase in air pollution, along a similar trajectory to that previously experienced by the developed nations. In China, particulate pollution is a serious environmental problem that is influencing air quality, regional and global climates, and human health. In response to the extremely severe and persistent haze pollution experienced by about 800 million people during the first quarter of 2013 (refs 4, 5), the Chinese State Council announced its aim to reduce concentrations of PM2.5 (particulate matter with an aerodynamic diameter less than 2.5 micrometres) by up to 25 per cent relative to 2012 levels by 2017 (ref. 6). Such efforts however require elucidation of the factors governing the abundance and composition of PM2.5, which remain poorly constrained in China. Here we combine a comprehensive set of novel and state-of-the-art offline analytical approaches and statistical techniques to investigate the chemical nature and sources of particulate matter at urban locations in Beijing, Shanghai, Guangzhou and Xi'an during January 2013. We find that the severe haze pollution event was driven to a large extent by secondary aerosol formation, which contributed 30-77 per cent and 44-71 per cent (average for all four cities) of PM2.5 and of organic aerosol, respectively. On average, the contribution of secondary organic aerosol (SOA) and secondary inorganic aerosol (SIA) are found to be of similar importance (SOA/SIA ratios range from 0.6 to 1.4). Our results suggest that, in addition to mitigating primary particulate emissions, reducing the emissions of secondary aerosol precursors from, for example, fossil fuel combustion and biomass burning is likely to be important for controlling China's PM2.5 levels and for reducing the environmental, economic and health impacts resulting from particulate pollution.