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Agricultural and prescribed burning activities emit large amounts of trace gases and aerosols on regional to global scales. We present a compilation of emission factors (EFs) and emission ratios (ERs) from the eastern portion of the Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) campaign in 2019 in the United States, which sampled burning of crop residues and other prescribed fire fuels. FIREX-AQ provided comprehensive chemical characterization of 53 crop residue and 22 prescribed fires. Crop residues burned at different modified combustion efficiencies (MCE), with corn residue burning at higher MCE than other fuel types. Prescribed fires burned at lower MCE (<0.90) which is typical, while grasslands burned at lower MCE (0.90) than normally observed due to moist, green, growing season fuels. Most non-methane volatile organic compounds (NMVOCs) were significantly anticorrelated with MCE except for ethanol and NMVOCs that were measured with less certainty. We identified 23 species where crop residue fires differed by more than 50% from prescribed fires at the same MCE. Crop residue EFs were greater for species related to agricultural chemical use and fuel composition as well as oxygenated NMVOCs possibly due to the presence of metals such as potassium. Prescribed EFs were greater for monoterpenes (5×). FIREX-AQ crop residue average EFs generally agreed with the previous agricultural fire study in the US but had large disagreements with global compilations. FIREX-AQ observations show the importance of regionally-specific and fuel-specific EFs as first steps to reduce uncertainty in modeling the air quality impacts of fire emissions.

The NOAA/NASA Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) experiment was a multi-agency, inter-disciplinary research effort to: (a) obtain detailed measurements of trace gas and aerosol emissions from wildfires and prescribed fires using aircraft, satellites and ground-based instruments, (b) make extensive suborbital remote sensing measurements of fire dynamics, (c) assess local, regional, and global modeling of fires, and (d) strengthen connections to observables on the ground such as fuels and fuel consumption and satellite products such as burned area and fire radiative power. From Boise, ID western wildfires were studied with the NASA DC-8 and two NOAA Twin Otter aircraft. The high-altitude NASA ER-2 was deployed from Palmdale, CA to observe some of these fires in conjunction with satellite overpasses and the other aircraft. Further research was conducted on three mobile laboratories and ground sites, and 17 different modeling forecast and analyses products for fire, fuels and air quality and climate implications. From Salina, KS the DC-8 investigated 87 smaller fires in the Southeast with remote and in-situ data collection. Sampling by all platforms was designed to measure emissions of trace gases and aerosols with multiple transects to capture the chemical transformation of these emissions and perform remote sensing observations of fire and smoke plumes under day and night conditions. The emissions were linked to fuels consumed and fire radiative power using orbital and suborbital remote sensing observations collected during overflights of the fires and smoke plumes and ground sampling of fuels.

High levels of fine particulate matter (PM2.5) pollution in East Asia often exceed local air quality standards. Observations from the Korea United States-Air Quality (KORUS-AQ) field campaign in May and June 2016 showed that development of extreme pollution (haze) occurred through a combination of long-range transport and favorable meteorological conditions that enhanced local production of PM2.5. Atmospheric models often have difficulty simulating PM2.5 chemical composition during haze, which is of concern for the development of successful control measures. We use observations from KORUS-AQ to examine the ability of the GEOS-Chem chemical transport model to simulate PM2.5 composition throughout the campaign and identify the mechanisms driving the pollution event. At the surface, the model underestimates sulfate by -64% but overestimates nitrate by +36%. The largest underestimate in sulfate occurs during the pollution event, where models typically struggle to generate elevated sulfate concentrations due to missing heterogeneous chemistry in aerosol liquid water in the polluted boundary layer. Hourly surface observations show that the model nitrate bias is driven by an overestimation of the nighttime peak. In the model, nitrate formation is limited by the supply of nitric acid, which is biased by +100% against aircraft observations. We hypothesize that this is due to a large missing sink, which we implement here as a factor of five increase in dry deposition. We show that the resulting increased deposition velocity is consistent with observations of total nitrate as a function of photochemical age. The model does not account for factors such as the urban heat island effect or the heterogeneity of the built-up urban landscape resulting in insufficient model turbulence and surface area over the study area that likely results in insufficient dry deposition. Other species such as NH3 could be similarly affected but were not measured during the campaign. Nighttime production of nitrate is driven by NO2 hydrolysis in the model, while observations show that unexpectedly elevated nighttime ozone (not present in the model) should result in N2O5 hydrolysis as the primary pathway. The model is unable to represent nighttime ozone due to an overly rapid collapse of the afternoon mixed layer and excessive titration by NO. We attribute this to missing nighttime heating driving deeper nocturnal mixing that would be expected to occur in a city like Seoul. This urban heating is not considered in air quality models run at large enough scales to treat both local chemistry and long-range transport. Key model failures in simulating nitrate, mainly overestimated daytime nitric acid, incorrect representation of nighttime chemistry, and an overly shallow and insufficiently turbulent nighttime mixed layer, exacerbate the model’s inability to simulate the buildup of PM2.5 during haze pollution. To address the underestimate in sulfate most evident during the haze event, heterogeneous aerosol uptake of SO2 is added to the model which previously only considered aqueous production of sulfate from SO2 in cloud water. Implementing a simple parameterization of this chemistry improves the model abundance of sulfate but degrades the SO2 simulation implying that emissions are underestimated. We find that improving model simulations of sulfate has direct relevance to determining local vs. transboundary contributions to PM2.5. During the haze pollution event, the inclusion of heterogeneous aerosol uptake of SO2 decreases the fraction of PM2.5 attributable to long-range transport from 66% to 54%. Locally-produced sulfate increased from 1% to 25% of locally-produced PM2.5, implying that local emissions controls would have a larger effect than previously thought. However, this additional uptake of SO2 is coupled to the model nitrate prediction which affects the aerosol liquid water abundance and chemistry driving sulfate-nitrate-ammonium partitioning. An additional simulation of the haze pollution with heterogeneous uptake of SO2 to aerosol and simple improvements to the model nitrate simulation results in 30% less sulfate due to 40% less nitrate and aerosol water, and results in an underestimate of sulfate during the haze event. Future studies need to better consider the impact of model physical processes such as dry deposition and nighttime boundary layer mixing on the simulation of nitrate and the effect of improved nitrate simulations on the overall simulation of secondary inorganic aerosol (sulfate+nitrate+ammonium) in East Asia. Foreign emissions are rapidly changing, increasing the need to understand the impact of local emissions on PM2.5 in South Korea to ensure continued air quality improvements.

Ozone (O3) dry deposition is a major O3 sink. As a follow-up study of Huang et al. (2021), we quantify the impact of satellite soil moisture (SM) on model representations of this process when different dry-deposition parameterizations are implemented, based on which the implications for interpreting O3 air pollution levels and assessing the O3 impacts on human and ecosystem health are provided. The SM data from NASA's Soil Moisture Active Passive mission are assimilated into the Noah-Multiparameterization (Noah-MP) land surface model within the NASA Land Information System framework, semicoupled with Weather Research and Forecasting model with online Chemistry (WRF-Chem) regional-scale simulations covering the southeastern US. Major changes in the modeling system used include enabling the dynamic vegetation option, adding the irrigation process, and updating the scheme for the surface exchange coefficient. Two dry-deposition schemes are implemented, i.e., the Wesely scheme and a “dynamic” scheme, in the latter of which dry-deposition parameterization is coupled with photosynthesis and vegetation dynamics. It is demonstrated that, when the dynamic scheme is applied, the simulated O3 dry-deposition velocities vd and their stomatal and cuticular portions, as well as the total O3 fluxes Ft, are larger overall; vd and Ft are 2–3 times more sensitive to the SM changes due to the data assimilation (DA). Further, through case studies at two forested sites with different soil types and hydrological regimes, we highlight that, applying the Community Land Model type of SM factor controlling stomatal resistance (i.e., β factor) scheme in replacement of the Noah-type β factor scheme reduced the v(d) sensitivity to SM changes by ∼75 % at one site, while it doubled this sensitivity at the other site. Referring to multiple evaluation datasets, which may be associated with variable extents of uncertainty, the model performance of vegetation, surface fluxes, weather, and surface O3 concentrations shows mixed responses to the DA, some of which display land cover dependency. Finally, using model-derived concentration- and flux-based policy-relevant O3 metrics as well as their matching exposure–response functions, the relative biomass/crop yield losses for several types of vegetation/crops are estimated to be within a wide range of 1 %–17 %. Their sensitivities to the model's dry-deposition scheme and the implementation of SM DA are discussed.

Radon-222 (Rn-222) is a short-lived radioactive gas naturally emitted from land surfaces and has long been used to assess convective transport in atmospheric models. In this study, we simulate Rn-222 using the GEOS-Chem chemical transport model to improve our understanding of Rn-222 emissions and surface concentration seasonality and characterize convective transport associated with two Goddard Earth Observing System (GEOS) meteorological products, the Modern-Era Retrospective analysis for Research and Applications (MERRA) and GEOS Forward Processing (GEOS-FP). We evaluate four global Rn-222 emission scenarios by comparing model results with observations at 51 surface sites. The default emission scenario in GEOS-Chem yields a moderate agreement with surface observations globally (68.9 % of data within a factor of 2) and a large underestimate of winter surface Rn-222 concentrations at Northern Hemisphere midlatitudes and high latitudes due to an oversimplified formulation of Rn-222 emission fluxes (1 atom cm−2 s−1 over land with a reduction by a factor of 3 under freezing conditions). We compose a new global Rn-222 emission scenario based on Zhang et al. (2011) and demonstrate its potential to improve simulated surface Rn-222 concentrations and seasonality. The regional components of this scenario include spatially and temporally varying emission fluxes derived from previous measurements of soil radium content and soil exhalation models, which are key factors in determining Rn-222 emission flux rates. However, large model underestimates of surface Rn-222 concentrations still exist in Asia, suggesting unusually high regional Rn-222 emissions. We therefore propose a conservative upscaling factor of 1.2 for Rn-222 emission fluxes in China, which was also constrained by observed deposition fluxes of 210Pb (a progeny of Rn-222). With this modification, the model shows better agreement with observations in Europe and North America (> 80 % of data within a factor of 2) and reasonable agreement in Asia (close to 70 %). Further constraints on Rn-222 emissions would require additional concentration and emission flux observations in the central United States, Canada, Africa, and Asia. We also compare and assess convective transport in model simulations driven by MERRA and GEOS-FP using observed Rn-222 vertical profiles in northern midlatitude summer and from three short-term airborne campaigns. While simulations with both GEOS products are able to capture the observed vertical gradient of Rn-222 concentrations in the lower troposphere (0–4 km), neither correctly represents the level of convective detrainment, resulting in biases in the middle and upper troposphere. Compared with GEOS-FP, MERRA leads to stronger convective transport of Rn-222, which is partially compensated for by its weaker large-scale vertical advection, resulting in similar global vertical distributions of Rn-222 concentrations between the two simulations. This has important implications for using chemical transport models to interpret the transport of other trace species when these GEOS products are used as driving meteorology.

Satellite ammonia (NH3) observations provide unprecedented insights into NH3 emissions, spatiotemporal variabilities and trends, but validation with in situ measurements remains lacking. Here, total columns from the Infrared Atmospheric Sounding Interferometer (IASI) were intercompared to boundary layer NH3 profiles derived from aircraft- and surface-based measurements primarily in Colorado, USA, in the summer of 2014. IASI-NH3 version 3 near real-time data set compared well to in situ derived columns (windows ±15 km around centroid, ±1 h around overpass time) with a correlation of 0.58, a slope of 0.78 ± 0.14 and an intercept of 2.1 × 1015±1.5 × 1015 molecules cm−2. Agreement degrades at larger spatiotemporal windows, consistent with the short atmospheric lifetime of NH3. We also examined IASI version 3R data, which relies on temperature retrievals from the ERA Reanalysis, and a third product generated using aircraft-measured temperature profiles. The overall agreement improves slightly for both cases, and neither is biased within their combined measurement errors. Thus, spatiotemporal averaging of IASI over large windows can be used to reduce retrieval noise. Nonetheless, sampling artifacts of airborne NH3 instruments result in significant uncertainties of the in situ-derived columns. For example, large validation differences exist between ascent and descent profiles, and the assumptions of the free tropospheric NH3 profiles used above the aircraft ceiling significantly impact the validation. Because short-lived species like NH3 largely reside within the boundary layer with complex vertical structures, more comprehensive validation is needed across a wide range of environments. More accurate and widespread in situ NH3 data sets are therefore required for improved validations of satellite products.

KORUS-AQ was an international cooperative air quality field study in South Korea that measured local and remote sources of air pollution affecting the Korean Peninsula during May–June 2016. Some of the largest aerosol mass concentrations were measured during a Chinese haze transport event (24 May). Air quality forecasts using the WRF-Chem model with aerosol optical depth (AOD) data assimilation captured AOD during this pollution episode but overpredicted surface particulate matter concentrations in South Korea, especially PM2.5, often by a factor of 2 or larger. Analysis revealed multiple sources of model deficiency related to the calculation of optical properties from aerosol mass that explain these discrepancies. Using in situ observations of aerosol size and composition as inputs to the optical properties calculations showed that using a low-resolution size bin representation (four bins) underestimates the efficiency with which aerosols scatter and absorb light (mass extinction efficiency). Besides using finer-resolution size bins (8–16 bins), it was also necessary to increase the refractive indices and hygroscopicity of select aerosol species within the range of values reported in the literature to achieve better consistency with measured values of the mass extinction efficiency (6.7 m2 g−1 observed average) and light-scattering enhancement factor (f(RH)) due to aerosol hygroscopic growth (2.2 observed average). Furthermore, an evaluation of the optical properties obtained using modeled aerosol properties revealed the inability of sectional and modal aerosol representations in WRF-Chem to properly reproduce the observed size distribution, with the models displaying a much wider accumulation mode. Other model deficiencies included an underestimate of organic aerosol density (1.0 g cm−3 in the model vs. observed average of 1.5 g cm−3) and an overprediction of the fractional contribution of submicron inorganic aerosols other than sulfate, ammonium, nitrate, chloride, and sodium corresponding to mostly dust (17 %–28 % modeled vs. 12 % estimated from observations). These results illustrate the complexity of achieving an accurate model representation of optical properties and provide potential solutions that are relevant to multiple disciplines and applications such as air quality forecasts, health impact assessments, climate projections, solar power forecasts, and aerosol data assimilation.