Sulfur dioxide (SO₂) measurements from the Ozone Monitoring Instrument (OMI) satellite sensor processed with the new principal component analysis (PCA) algorithm were used to detect large point emission sources or clusters of sources. The total of 491 continuously emitting point sources releasing from about 30 kt yr⁻¹ to more than 4000 kt yr⁻¹ of SO₂ per year have been identified and grouped by country and by primary source origin: volcanoes (76 sources); power plants (297); smelters (53); and sources related to the oil and gas industry (65). The sources were identified using different methods, including through OMI measurements themselves applied to a new emission detection algorithm, and their evolution during the 2005–2014 period was traced by estimating annual emissions from each source. For volcanic sources, the study focused on continuous degassing, and emissions from explosive eruptions were excluded. Emissions from degassing volcanic sources were measured, many for the first time, and collectively they account for about 30 % of total SO₂ emissions estimated from OMI measurements, but that fraction has increased in recent years given that cumulative global emissions from power plants and smelters are declining while emissions from oil and gas industry remained nearly constant. Anthropogenic emissions from the USA declined by 80 % over the 2005–2014 period as did emissions from western and central Europe, whereas emissions from India nearly doubled, and emissions from other large SO₂-emitting regions (South Africa, Russia, Mexico, and the Middle East) remained fairly constant. In total, OMI-based estimates account for about a half of total reported anthropogenic SO₂ emissions; the remaining half is likely related to sources emitting less than 30 kt yr⁻¹ and not detected by OMI.

This study, performed under the umbrella of the Task Force on Hemispheric Transport of Air Pollution (TF-HTAP), responds to the global and regional atmospheric modelling community's need of a mosaic emission inventory of air pollutants that conforms to specific requirements: global coverage, long time series, spatially distributed emissions with high time resolution, and a high sectoral resolution. The mosaic approach of integrating official regional emission inventories based on locally reported data, with a global inventory based on a globally consistent methodology, allows modellers to perform simulations of high scientific quality while also ensuring that the results remain relevant to policymakers. HTAP_v3, an ad hoc global mosaic of anthropogenic inventories, has been developed by integrating official inventories over specific areas (North America, Europe, Asia including Japan and South Korea) with the independent Emissions Database for Global Atmospheric Research (EDGAR) inventory for the remaining world regions. The results are spatially and temporally distributed emissions of SO₂, NO_x, CO, non-methane volatile organic compounds (NMVOCs), NH₃, PM₁₀, PM_2.5, black carbon (BC), and organic carbon (OC), with a spatial resolution of 0.1^∘ × 0.1^∘ and time intervals of months and years, covering the period 2000–2018 (https://doi.org/10.5281/zenodo.7516361, Crippa, 2023, https://edgar.jrc.ec.europa.eu/dataset_htap_v3, last access: June 2023). The emissions are further disaggregated into 16 anthropogenic emitting sectors. This paper describes the methodology applied to develop such an emission mosaic, reports on source allocation, differences among existing inventories, and best practices for the mosaic compilation. One of the key strengths of the HTAP_v3 emission mosaic is its temporal coverage, enabling the analysis of emission trends over the past 2 decades. The development of a global emission mosaic over such long time series represents a unique product for global air quality modelling and for better-informed policymaking, reflecting the community effort expended by the TF-HTAP to disentangle the complexity of transboundary transport of air pollution.

Estimates of potential harmful effects on ecosystems in the Canadian provinces of Alberta and Saskatchewan due to acidifying deposition were calculated, using a 1-year simulation of a high-resolution implementation of the Global Environmental Multiscale-Modelling Air-quality and Chemistry (GEM-MACH) model, and estimates of aquatic and terrestrial ecosystem critical loads. The model simulation was evaluated against two different sources of deposition data: total deposition in precipitation and total deposition to snowpack in the vicinity of the Athabasca oil sands. The model captured much of the variability of observed ions in wet deposition in precipitation (observed versus model sulfur, nitrogen and base cation R² values of 0.90, 0.76 and 0.72, respectively), while being biased high for sulfur deposition, and low for nitrogen and base cations (slopes 2.2, 0.89 and 0.40, respectively). Aircraft-based estimates of fugitive dust emissions, shown to be a factor of 10 higher than reported to national emissions inventories (Zhang et al., 2018), were used to estimate the impact of increased levels of fugitive dust on model results. Model comparisons to open snowpack observations were shown to be biased high, but in reasonable agreement for sulfur deposition when observations were corrected to account for throughfall in needleleaf forests. The model–observation relationships for precipitation deposition data, along with the expected effects of increased (unreported) base cation emissions, were used to provide a simple observation-based correction to model deposition fields. Base cation deposition was estimated using published observations of base cation fractions in surface-collected particles (Wang et al., 2015). Both original and observation-corrected model estimates of sulfur, nitrogen, and base cation deposition were used in conjunction with critical load data created using the NEG-ECP (2001) and CLRTAP (2017) methods for calculating critical loads, using variations on the Simple Mass Balance model for terrestrial ecosystems, and the Steady State Water Chemistry and First-order Acidity Balance models for aquatic ecosystems. Potential ecosystem damage was predicted within each of the regions represented by the ecosystem critical load datasets used here, using a combination of 2011 and 2013 emissions inventories. The spatial extent of the regions in exceedance of critical loads varied between 1 × 10⁴ and 3.3 × 10⁵ km², for the more conservative observation-corrected estimates of deposition, with the variation dependent on the ecosystem and critical load calculation methodology. The larger estimates (for aquatic ecosystems) represent a substantial fraction of the area of the provinces examined. Base cation deposition was shown to be sufficiently high in the region to have a neutralizing effect on acidifying deposition, and the use of the aircraft and precipitation observation-based corrections to base cation deposition resulted in reasonable agreement with snowpack data collected in the oil sands area. However, critical load exceedances calculated using both observations and observation-corrected deposition suggest that the neutralization effect is limited in spatial extent, decreasing rapidly with distance from emissions sources, due to the rapid deposition of emitted primary dust particles as a function of their size. We strongly recommend the use of observation-based correction of model-simulated deposition in estimating critical load exceedances, in future work.

Despite its clear importance, the monitoring of atmospheric ammonia, including its sources, sinks, and links to the greater nitrogen cycle, remains limited. Satellite data are helping to fill the gap in monitoring from sporadic conventional ground- and aircraft-based observations to better inform policymakers and assess the impact of any ammonia-related policies. Presented is a description and survey that demonstrate the capabilities of the Cross-track Infrared Sounder (CrIS) ammonia product for monitoring, air quality forecast model evaluation, dry deposition estimates, and emission estimates from an agricultural hotspot. For model evaluation, while there is a general agreement in the spatial allocation of known major agricultural ammonia hotspots across North America, the satellite observations show some high-latitude regions during peak forest fire activity often have ammonia concentrations approaching those in agricultural hotspots. The CrIS annual ammonia dry depositions in Canada (excluding the territories) and the US have average and annual variability values of $\sim \mathrm{0.8}\pm \mathrm{0.08}$ and $\sim \mathrm{1.23}\pm \mathrm{0.09}$ Tg N yr⁻¹, respectively. These satellite-derived dry depositions of reactive nitrogen from NH₃ with NO₂ show an annual ratio of NH₃ compared to their sum (NH₃+NO₂) of ∼82 % and ∼55 % in Canada and the US, respectively. Furthermore, we show the use of CrIS satellite observations to estimate annual and seasonal emissions near Lethbridge, Alberta, Canada, a region dominated by high-emission concentrated animal feeding operations (CAFOs); the satellite annual emission estimate of 37.1±6.3 kt yr⁻¹ is at least double the value reported in current bottom-up emission inventories for this region.

We quantify methane emissions and their 2010–2017 trends by sector in the contiguous United States (CONUS), Canada, and Mexico by inverse analysis of in situ (GLOBALVIEWplus CH₄ ObsPack) and satellite (GOSAT) atmospheric methane observations. The inversion uses as a prior estimate the national anthropogenic emission inventories for the three countries reported by the US Environmental Protection Agency (EPA), Environment and Climate Change Canada (ECCC), and the Instituto Nacional de Ecología y Cambio Climático (INECC) in Mexico to the United Nations Framework Convention on Climate Change (UNFCCC) and thus serves as an evaluation of these inventories in terms of their magnitudes and trends. Emissions are optimized with a Gaussian mixture model (GMM) at $\mathrm{0.5}{}^{\circ }\times \mathrm{0.625}{}^{\circ }$ resolution and for individual years. Optimization is done analytically using lognormal error forms. This yields closed-form statistics of error covariances and information content on the posterior (optimized) estimates, allows better representation of the high tail of the emission distribution, and enables construction of a large ensemble of inverse solutions using different observations and assumptions. We find that GOSAT and in situ observations are largely consistent and complementary in the optimization of methane emissions for North America. Mean 2010–2017 anthropogenic emissions from our base GOSAT + in situ inversion, with ranges from the inversion ensemble, are 36.9 (32.5–37.8) Tg a⁻¹ for CONUS, 5.3 (3.6–5.7) Tg a⁻¹ for Canada, and 6.0 (4.7–6.1) Tg a⁻¹ for Mexico. These are higher than the most recent reported national inventories of 26.0 Tg a⁻¹ for the US (EPA), 4.0 Tg a⁻¹ for Canada (ECCC), and 5.0 Tg a⁻¹ for Mexico (INECC). The correction in all three countries is largely driven by a factor of 2 underestimate in emissions from the oil sector with major contributions from the south-central US, western Canada, and southeastern Mexico. Total CONUS anthropogenic emissions in our inversion peak in 2014, in contrast to the EPA report of a steady decreasing trend over 2010–2017. This reflects offsetting effects of increasing emissions from the oil and landfill sectors, decreasing emissions from the gas sector, and flat emissions from the livestock and coal sectors. We find decreasing trends in Canadian and Mexican anthropogenic methane emissions over the 2010–2017 period, mainly driven by oil and gas emissions. Our best estimates of mean 2010–2017 wetland emissions are 8.4 (6.4–10.6) Tg a⁻¹ for CONUS, 9.9 (7.8–12.0) Tg a⁻¹ for Canada, and 0.6 (0.4–0.6) Tg a⁻¹ for Mexico. Wetland emissions in CONUS show an increasing trend of +2.6 (+1.7 to +3.8)% a⁻¹ over 2010–2017 correlated with precipitation.

A parameter called the scavenging coefficient Λ is widely used in aerosol chemical transport models (CTMs) to describe below-cloud scavenging of aerosol particles by rain and snow. However, uncertainties associated with available size-resolved theoretical formulations for Λ span one to two orders of magnitude for rain scavenging and nearly three orders of magnitude for snow scavenging. Two recent reviews of below-cloud scavenging of size-resolved particles recommended that the upper range of the available theoretical formulations for Λ should be used in CTMs based on uncertainty analyses and comparison with limited field experiments. Following this recommended approach, a new semi-empirical parameterization for size-resolved Λ has been developed for below-cloud scavenging of atmospheric aerosol particles by both rain (Λ_rain) and snow (Λ_snow). The new parameterization is based on the 90th percentile of Λ values from an ensemble data set calculated using all possible "realizations" of available theoretical Λ formulas and covering a large range of aerosol particle sizes and precipitation intensities (R). For any aerosol particle size of diameter d, a strong linear relationship between the 90th-percentile log₁₀ (Λ) and log₁₀ (R), which is equivalent to a power-law relationship between Λ and R, is identified. The log-linear relationship, which is characterized by two parameters (slope and y intercept), is then further parameterized by fitting these two parameters as polynomial functions of aerosol size d. A comparison of the new parameterization with limited measurements in the literature in terms of the magnitude of Λ and the relative magnitudes of Λ_rain and Λ_snow suggests that it is a reasonable approximation. Advantages of this new semi-empirical parameterization compared to traditional theoretical formulations for Λ include its applicability to below-cloud scavenging by both rain and snow over a wide range of particle sizes and precipitation intensities, ease of implementation in any CTM with a representation of size-distributed particulate matter, and a known representativeness, based on the consideration in its development, of all available theoretical formulations and field-derived estimates for Λ (d) and their associated uncertainties.