Acidity, defined as pH, is a central component of aqueous chemistry. In the atmosphere, the acidity of condensed phases (aerosol particles, cloud water, and fog droplets) governs the phase partitioning of semivolatile gases such as HNO₃, NH₃, HCl, and organic acids and bases as well as chemical reaction rates. It has implications for the atmospheric lifetime of pollutants, deposition, and human health. Despite its fundamental role in atmospheric processes, only recently has this field seen a growth in the number of studies on particle acidity. Even with this growth, many fine-particle pH estimates must be based on thermodynamic model calculations since no operational techniques exist for direct measurements. Current information indicates acidic fine particles are ubiquitous, but observationally constrained pH estimates are limited in spatial and temporal coverage. Clouds and fogs are also generally acidic, but to a lesser degree than particles, and have a range of pH that is quite sensitive to anthropogenic emissions of sulfur and nitrogen oxides, as well as ambient ammonia. Historical measurements indicate that cloud and fog droplet pH has changed in recent decades in response to controls on anthropogenic emissions, while the limited trend data for aerosol particles indicate acidity may be relatively constant due to the semivolatile nature of the key acids and bases and buffering in particles. This paper reviews and synthesizes the current state of knowledge on the acidity of atmospheric condensed phases, specifically particles and cloud droplets. It includes recommendations for estimating acidity and pH, standard nomenclature, a synthesis of current pH estimates based on observations, and new model calculations on the local and global scale.

Various approaches have been proposed to model PM2.5 in the recent decade, with satellite-derived aerosol optical depth, land-use variables, chemical transport model predictions, and several meteorological variables as major predictor variables. Our study used an ensemble model that integrated multiple machine learning algorithms and predictor variables to estimate daily PM2.5 at a resolution of 1 km × 1 km across the contiguous United States. We used a generalized additive model that accounted for geographic difference to combine PM2.5 estimates from neural network, random forest, and gradient boosting. The three machine learning algorithms were based on multiple predictor variables, including satellite data, meteorological variables, land-use variables, elevation, chemical transport model predictions, several reanalysis datasets, and others. The model training results from 2000 to 2015 indicated good model performance with a 10-fold cross-validated R2 of 0.86 for daily PM2.5 predictions. For annual PM2.5 estimates, the cross-validated R2 was 0.89. Our model demonstrated good performance up to 60 μg/m3. Using trained PM2.5 model and predictor variables, we predicted daily PM2.5 from 2000 to 2015 at every 1 km × 1 km grid cell in the contiguous United States. We also used localized land-use variables within 1 km × 1 km grids to downscale PM2.5 predictions to 100 m × 100 m grid cells. To characterize uncertainty, we used meteorological variables, land-use variables, and elevation to model the monthly standard deviation of the difference between daily monitored and predicted PM2.5 for every 1 km × 1 km grid cell. This PM2.5 prediction dataset, including the downscaled and uncertainty predictions, allows epidemiologists to accurately estimate the adverse health effect of PM2.5. Compared with model performance of individual base learners, an ensemble model would achieve a better overall estimation. It is worth exploring other ensemble model formats to synthesize estimations from different models or from different groups to improve overall performance.

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.

Information on the deposition efficiency of aerosol particles in the nasal airways is used for optimizing the delivery of therapeutic aerosols into the nose and for risk assessment of toxic airborne pollutants inhaled through the nose into the respiratory system. Nasal particle deposition is often studied using plastic replicas of nasal airways. Deposition efficiency in a nasal replica manufactured by stereolithography has not been reported to date. We determined the inertial particle deposition efficiency of two replicas of the same nasal airways manufactured by different stereolithography machines and compared results with deposition efficiencies reported for models manufactured by other techniques from the same magnetic resonance imaging scans. Deposition in the replicas was measured for particles of aerodynamic diameter between 1 and 10 μm and constant inspiratory flow rates ranging from 20–40 Ipm. Deposition efficiency of the replicas increased from nearly 0–100% with increasing particle inertia. For a range of particle inertias, particle deposition in the replica made with higher resolution stereolithography machine was slightly less than in the replica made with a lower resolution stereolithography process. These data showed lower deposition efficiency when compared with other deposition studies in nasal replicas based on the same magnetic resonance imaging data. The differences in deposition efficiency can be attributed in part to differences in methods used to manufacture the replicas. There was little or no difference in deposition due to cutting tool size, some difference due to the use of assembly plates, and some difference due to surface roughness. These associations suggest that inertial nasal particle deposition is significantly influenced by small differences in nasal airways.