Existing descriptions of bi-directional ammonia (NH ₃ ) land–atmosphere exchange incorporate temperature and moisture controls, and are beginning to be used in regional chemical transport models. However, such models have typically applied simpler emission factors to upscale the main NH ₃ emission terms. While this approach has successfully simulated the main spatial patterns on local to global scales, it fails to address the environment- and climate-dependence of emissions. To handle these issues, we outline the basis for a new modelling paradigm where both NH ₃ emissions and deposition are calculated online according to diurnal, seasonal and spatial differences in meteorology. We show how measurements reveal a strong, but complex pattern of climatic dependence, which is increasingly being characterized using ground-based NH ₃ monitoring and satellite observations, while advances in process-based modelling are illustrated for agricultural and natural sources, including a global application for seabird colonies. A future architecture for NH ₃ emission–deposition modelling is proposed that integrates the spatio-temporal interactions, and provides the necessary foundation to assess the consequences of climate change. Based on available measurements, a first empirical estimate suggests that 5°C warming would increase emissions by 42 per cent (28–67%). Together with increased anthropogenic activity, global NH ₃ emissions may increase from 65 (45–85) Tg N in 2008 to reach 132 (89–179) Tg by 2100.

The Community Multiscale Air Quality (CMAQ) model version 5.3 (CMAQ53), released to the public in August 2019 and followed by version 5.3.1 (CMAQ531) in December 2019, contains numerous science updates, enhanced functionality, and improved computation efficiency relative to the previous version of the model, 5.2.1 (CMAQ521). Major science advances in the new model include a new aerosol module (AERO7) with significant updates to secondary organic aerosol (SOA) chemistry, updated chlorine chemistry, updated detailed bromine and iodine chemistry, updated simple halogen chemistry, the addition of dimethyl sulfide (DMS) chemistry in the CB6r3 chemical mechanism, updated M3Dry bidirectional deposition model, and the new Surface Tiled Aerosol and Gaseous Exchange (STAGE) bidirectional deposition model. In addition, support for the Weather Research and Forecasting (WRF) model's hybrid vertical coordinate (HVC) was added to CMAQ53 and the Meteorology-Chemistry Interface Processor (MCIP) version 5.0 (MCIP50). Enhanced functionality in CMAQ53 includes the new Detailed Emissions Scaling, Isolation and Diagnostic (DESID) system for scaling incoming emissions to CMAQ and reading multiple gridded input emission files. Evaluation of CMAQ531 was performed by comparing monthly and seasonal mean daily 8 h average (MDA8) O₃ and daily PM_2.5 values from several CMAQ531 simulations to a similarly configured CMAQ521 simulation encompassing 2016. For MDA8 O₃, CMAQ531 has higher O₃ in the winter versus CMAQ521, due primarily to reduced dry deposition to snow, which strongly reduces wintertime O₃ bias (2–4 ppbv monthly average). MDA8 O₃ is lower with CMAQ531 throughout the rest of the year, particularly in spring, due in part to reduced O₃ from the lateral boundary conditions (BCs), which generally increases MDA8 O₃ bias in spring and fall (∼0.5 µg m⁻³). For daily 24 h average PM_2.5, CMAQ531 has lower concentrations on average in spring and fall, higher concentrations in summer, and similar concentrations in winter to CMAQ521, which slightly increases bias in spring and fall and reduces bias in summer. Comparisons were also performed to isolate updates to several specific aspects of the modeling system, namely the lateral BCs, meteorology model version, and the deposition model used. Transitioning from a hemispheric CMAQ (HCMAQ) version 5.2.1 simulation to a HCMAQ version 5.3 simulation to provide lateral BCs contributes to higher O₃ mixing ratios in the regional CMAQ simulation in higher latitudes during winter (due to the decreased O₃ dry deposition to snow in CMAQ53) and lower O₃ mixing ratios in middle and lower latitudes year-round (due to reduced O₃ over the ocean with CMAQ53). Transitioning from WRF version 3.8 to WRF version 4.1.1 with the HVC resulted in consistently higher (1.0–1.5 ppbv) MDA8 O₃ mixing ratios and higher PM_2.5 concentrations (0.1–0.25 µg m⁻³) throughout the year. Finally, comparisons of the M3Dry and STAGE deposition models showed that MDA8 O₃ is generally higher with M3Dry outside of summer, while PM_2.5 is consistently higher with STAGE due to differences in the assumptions of particle deposition velocities to non-vegetated surfaces and land use with short vegetation (e.g., grasslands) between the two models. For ambient NH₃, STAGE has slightly higher concentrations and smaller bias in the winter, spring, and fall, while M3Dry has higher concentrations and smaller bias but larger error and lower correlation in the summer.

We use the adjoint of a global 3‐D chemical transport model (GEOS‐Chem) to optimize ammonia (NH₃) emissions in the U.S., European Union, and China by inversion of 2005–2008 network data forwet deposition fluxes. Optimized emissions are derived on a 2° × 2.5° grid for individual months and years. Error characterization in the optimization includes model errors in precipitation. Annual optimized emissions are 2.8 Tg NH₃−N a⁻¹for the contiguous U.S., 3.1 Tg NH₃−N a⁻¹for the European Union, and 8.4 Tg NH₃−N a⁻¹for China. Comparisons to previous inventories for the U.S. and European Union show consistency (∼±15%) in annual totals but some large spatial and seasonal differences. We develop a new global bottom‐up inventory of NH₃emissions (Magnitude And Seasonality of Agricultural Emissions model for NH3 (MASAGE_NH3)) to interpret the results of the adjoint optimization. MASAGE_NH3 provides information on the magnitude and seasonality of NH₃emissions from individual crop and livestock sources on a 0.5° × 0.5° grid. We find that U.S. emissions peak in the spring in the Midwest due to corn fertilization and in the summer elsewhere due to manure. The seasonality of European emissions is more homogeneous with a well‐defined maximum in spring associated with manure and mineral fertilizer application. There is some evidence for the effect of European regulations of NH₃emissions, notably a large fall decrease in northern Europe. Emissions in China peak in summer because of the summertime application of fertilizer for double cropping.

This paper describes the scientific and structural updates to the latest release of the Community Multiscale Air Quality (CMAQ) modeling system version 4.7 (v4.7) and points the reader to additional resources for further details. The model updates were evaluated relative to observations and results from previous model versions in a series of simulations conducted to incrementally assess the effect of each change. The focus of this paper is on five major scientific upgrades: (a) updates to the heterogeneous N₂O₅ parameterization, (b) improvement in the treatment of secondary organic aerosol (SOA), (c) inclusion of dynamic mass transfer for coarse-mode aerosol, (d) revisions to the cloud model, and (e) new options for the calculation of photolysis rates. Incremental test simulations over the eastern United States during January and August 2006 are evaluated to assess the model response to each scientific improvement, providing explanations of differences in results between v4.7 and previously released CMAQ model versions. Particulate sulfate predictions are improved across all monitoring networks during both seasons due to cloud module updates. Numerous updates to the SOA module improve the simulation of seasonal variability and decrease the bias in organic carbon predictions at urban sites in the winter. Bias in the total mass of fine particulate matter (PM_2.5) is dominated by overpredictions of unspeciated PM_2.5 (PM_other) in the winter and by underpredictions of carbon in the summer. The CMAQv4.7 model results show slightly worse performance for ozone predictions. However, changes to the meteorological inputs are found to have a much greater impact on ozone predictions compared to changes to the CMAQ modules described here. Model updates had little effect on existing biases in wet deposition predictions.

The Community Multiscale Air Quality (CMAQ) model is a comprehensive multipollutant air quality modeling system developed and maintained by the US Environmental Protection Agency's (EPA) Office of Research and Development (ORD). Recently, version 5.1 of the CMAQ model (v5.1) was released to the public, incorporating a large number of science updates and extended capabilities over the previous release version of the model (v5.0.2). These updates include the following: improvements in the meteorological calculations in both CMAQ and the Weather Research and Forecast (WRF) model used to provide meteorological fields to CMAQ, updates to the gas and aerosol chemistry, revisions to the calculations of clouds and photolysis, and improvements to the dry and wet deposition in the model. Sensitivity simulations isolating several of the major updates to the modeling system show that changes to the meteorological calculations result in enhanced afternoon and early evening mixing in the model, periods when the model historically underestimates mixing. This enhanced mixing results in higher ozone (O₃) mixing ratios on average due to reduced NO titration, and lower fine particulate matter (PM_2. 5) concentrations due to greater dilution of primary pollutants (e.g., elemental and organic carbon). Updates to the clouds and photolysis calculations greatly improve consistency between the WRF and CMAQ models and result in generally higher O₃ mixing ratios, primarily due to reduced cloudiness and attenuation of photolysis in the model. Updates to the aerosol chemistry result in higher secondary organic aerosol (SOA) concentrations in the summer, thereby reducing summertime PM_2. 5 bias (PM_2. 5 is typically underestimated by CMAQ in the summer), while updates to the gas chemistry result in slightly higher O₃ and PM_2. 5 on average in January and July. Overall, the seasonal variation in simulated PM_2. 5 generally improves in CMAQv5.1 (when considering all model updates), as simulated PM_2. 5 concentrations decrease in the winter (when PM_2. 5 is generally overestimated by CMAQ) and increase in the summer (when PM_2. 5 is generally underestimated by CMAQ). Ozone mixing ratios are higher on average with v5.1 vs. v5.0.2, resulting in higher O₃ mean bias, as O₃ tends to be overestimated by CMAQ throughout most of the year (especially at locations where the observed O₃ is low); however, O₃ correlation is largely improved with v5.1. Sensitivity simulations for several hypothetical emission reduction scenarios show that v5.1 tends to be slightly more responsive to reductions in NO_x (NO + NO₂), VOC and SO_x (SO₂ + SO₄) emissions than v5.0.2, representing an improvement as previous studies have shown CMAQ to underestimate the observed reduction in O₃ due to large, widespread reductions in observed emissions.