Chemical Transport Model Simulations Research Articles

Capturing Exposure Disparities with Chemical Transport Models: Evaluating the Suitability of Downscaling Using Land Use Regression.

High resolution exposure surfaces are essential to capture disparities in exposure to traffic-related air pollution in urban areas. In this study, we develop an approach to downscale Chemical Transport Model (CTM) simulations to a hyperlocal level (∼100m) in the Greater Toronto Area (GTA) under three scenarios where emissions from cars, trucks and buses are zeroed out, thus capturing the burden of each transportation mode. This proposed approach statistically fuses CTMs with Land-Use Regression using machine learning techniques. With this proposed downscaling approach, changes in air pollutant concentrations under different scenarios are appropriately captured by downscaling factors that are trained to reflect the spatial distribution of emission reductions. Our validation analysis shows that high-resolution models resulted in better performance than coarse models when compared with observations at reference stations. We used this downscaling approach to assess disparities in exposure to nitrogen dioxide (NO2) for populations composed of renters, low-income households, recent immigrants, and visible minorities. Individuals in all four categories were disproportionately exposed to the burden of cars, trucks, and buses. We conducted this analysis at spatial resolutions of 12, 4, 1 km, and 100 m and observed that disparities were significantly underestimated when using coarse spatial resolutions. This reinforces the need for high-spatial resolution exposure surfaces for environmental justice analyses.

Can we reach consensus on the dominant sulfate formation pathway in China's haze?

Atmospheric sulfate aerosols contribute significantly to air pollution and climate change. Sulfate formation mechanisms during winter haze events in northern China have recently received considerable attention, with more than 10 studies published in high-impact journals. However, the conclusions from in-field measurements, laboratory studies, and numerical simulations are inconsistent and even contradictory. Here, we propose a physically based yet simple method to clarify the debate on the dominant sulfate formation pathway. Based on the hazes evolving in the synoptic scale, first, a characteristic sulfate formation rate is derived using the Eulerian mass conservation equation constrained by in situ observations. Then, this characteristic value is treated as a guideline to determine the dominant sulfate formation pathway with a 0D chemical box model. Our observation-derived results establish a linkage between studies from laboratory experiments and chemical transport model simulations. A convergent understanding could therefore be reached on sulfate formation mechanisms in China's wintertime haze. This method is universal and can be applied to various haze conditions and different secondary products.

Learned 1D Passive Scalar Advection to Accelerate Chemical Transport Modeling: A Case Study with GEOS-FP Horizontal Wind Fields

Abstract We developed and applied a machine-learned discretization for one-dimensional (1D) horizontal passive scalar advection, which is an operator component common to all chemical transport models (CTMs). Our learned advection scheme resembles a second-order accurate, three-stencil numerical solver but differs from a traditional solver in that coefficients for each equation term are output by a neural network rather than being theoretically derived constants. We subsampled higher-resolution simulation results—resulting in up to 16× larger grid size and 64× larger time step—and trained our neural-network-based scheme to match the subsampled integration data. In this way, we created an operator that has low resolution (in time or space) but can reproduce the behavior of a high-resolution traditional solver. Our model shows high fidelity in reproducing its training dataset (a single 10-day 1D simulation) and is similarly accurate in simulations with unseen initial conditions, wind fields, and grid spacing. In many cases, our learned solver is more accurate than a low-resolution version of the reference solver, but the low-resolution reference solver achieves greater computational speedup (500× acceleration) over the high-resolution simulation than the learned solver is able to (18× acceleration). Surprisingly, our learned 1D scheme—when combined with a splitting technique—can be used to predict 2D advection and is in some cases more stable and accurate than the low-resolution reference solver in 2D. Overall, our results suggest that learned advection operators may offer a higher-accuracy method for accelerating CTM simulations as compared to simply running a traditional integrator at low resolution. Significance Statement Chemical transport modeling (CTM) is an essential tool for studying air pollution. CTM simulations take a long computing time. Modeling pollutant transport (advection) is the second most computationally intensive part of the model. Decreasing the resolution not only reduces the advection computing time but also decreases accuracy. We employed machine learning to reduce the resolution of advection while keeping the accuracy. We verified the robustness of our solver with several generalization testing scenarios. In our 2D simulation, our solver showed up to 100 times faster simulation with fair accuracy. Integrating our approach to existing CTMs will allow broadened participation in the study of air pollution and related solutions.

Interpreting Geostationary Environment Monitoring Spectrometer (GEMS) geostationary satellite observations of the diurnal variation in nitrogen dioxide (NO2) over East Asia

Abstract. Nitrogen oxide radicals (NOx≡NO+NO2) emitted by fuel combustion are important precursors of ozone and particulate matter pollution, and NO2 itself is harmful to public health. The Geostationary Environment Monitoring Spectrometer (GEMS), launched in space in 2020, now provides hourly daytime observations of NO2 columns over East Asia. This diurnal variation offers unique information on the emission and chemistry of NOx, but it needs to be carefully interpreted. Here we investigate the drivers of the diurnal variation in NO2 observed by GEMS during winter and summer over Beijing and Seoul. We place the GEMS observations in the context of ground-based column observations (Pandora instruments) and GEOS-Chem chemical transport model simulations. We find good agreement between the diurnal variations in NO2 columns in GEMS, Pandora, and GEOS-Chem, and we use GEOS-Chem to interpret these variations. NOx emissions are 4 times higher in the daytime than at night, driving an accumulation of NO2 over the course of the day, offset by losses from chemistry and transport (horizontal flux divergence). For the urban core, where the Pandora instruments are located, we find that NO2 in winter increases throughout the day due to high daytime emissions and increasing NO2/NOx ratio from entrainment of ozone, partly balanced by loss from transport and with a negligible role of chemistry. In summer, by contrast, chemical loss combined with transport drives a minimum in the NO2 column at 13:00–14:00 local time (LT). Segregation of the GEMS data by wind speed further demonstrates the effect of transport, with NO2 in winter accumulating throughout the day at low winds but flat at high winds. The effect of transport can be minimized in summer by spatially averaging observations over the broader metropolitan scale, under which conditions the diurnal variation in NO2 reflects a dynamic balance between emission and chemical loss.

Short-Term Exposure to Fine Particulate Matter and Ozone: Source Impacts and Attributable Mortalities.

Short-term exposure to particles with aerodynamic diameters less than 2.5 μm (PM2.5) and ozone (O3) are important risk factors for human health. Despite the awareness of reducing attributable health burden, region-specific and source-specific strategies remain less explored due to the gap between precursor emissions and health effects. In this study, we isolate the health burden of individual sector sources of PM2.5 and O3 precursors, nitrogen oxides (NOx) and volatile organic compounds (VOCs), across the globe. Specifically, we estimate mortalities attributable to short-term exposure using machine-learning-based daily exposure estimates and quantify sectoral impacts using chemical transport model simulations. Globally, short-term exposure to PM2.5 and O3 result in 713.5 (95% Confidence Interval: 598.8-843.3) thousand and 496.3 (371.3-646.1) thousand mortalities in 2019, respectively, of which 12.5% are contributed by fuel-related NOx emissions from transportation, energy, and industry. Sectoral impacts from anthropogenic NOx and VOC emissions on health burden vary significantly among seasons and regions, requiring a target shift from transportation in winter to industry in summer for East Asia, for instance. Emission control and health management are additionally complicated by unregulated natural influences during climatic events. Fire-sourced NOx and VOC emissions, respectively, contribute to 8.5 (95% CI: 6.2-11.7) thousand and 4.8 (3.6-5.9) thousand PM2.5 and O3 mortalities, particularly for tropics with high vulnerability to climate change. Additionally, biogenic VOC emissions during heatwaves contribute to 1.8 (95% CI: 1.5-2.2) thousand O3-introduced mortalities, posing challenges in urban planning for high-income regions, where biogenic contributions to health burden during heatwaves are 13% of anthropogenic contributions annually. Our study provides important implications for temporally dynamic and sector-targeted emission control and health management strategies, which are of urgency under the projection of continuously increasing energy consumption and changing climate.

Satellite-based analysis of top of atmosphere shortwave radiative forcing trend induced by biomass burning aerosols over South-Eastern Atlantic

This study investigates long-term changes in the shortwave direct aerosol radiative effect (DARE) at the top of the atmosphere (TOA) induced by biomass burning aerosol (BBA) transported from southern Africa to the south-eastern Atlantic (SEA) stratocumulus region during extended fire seasons. The evolution since 2002 of aerosol, cloud properties, and TOA shortwave outgoing radiation from advanced passive satellite sensors are presented, as well as the observational trend in clear-sky DAREclr and the retrieval trend in all-sky DAREall. Supplemented by chemical transport model simulations, we estimate that DAREclr has become more negative (−0.09 ± 0.06 W m−2 yr−1) due to increased aerosol presence in SEA. Meanwhile, DAREall has become more positive ( + 0.04 ± 0.15 W m−2 yr−1) due to aerosols in cloudy sky regions. This study reveals satellite capabilities in capturing complex BBA-cloud-solar radiation interactions for accurate radiative forcing estimates and projections.

Investigating Zonal Asymmetries in Stratospheric Ozone Trends From Satellite Limb Observations and a Chemical Transport Model

AbstractThis study investigates the origin of a zonal asymmetry in stratospheric ozone trends at northern high latitudes, identified in satellite limb observations over the past two decades. We use a merged data set consisting of ozone profiles retrieved at the University of Bremen from SCIAMACHY and OMPS‐LP measurements to derive ozone trends. We also use TOMCAT chemical transport model (CTM) simulations, forced by ERA5 reanalyses, to investigate the factors that drive the asymmetry observed in the long‐term changes. By studying seasonally and longitudinally resolved observation‐based ozone trends, we find, especially during spring, a well‐pronounced asymmetry at polar latitudes with values up to +6 % per decade over Greenland and −5 % per decade over western Russia. The control CTM simulation agrees well with these observed trends, whereas sensitivity simulations indicate that chemical mechanisms involved in the production and removal of ozone, or their changes, are unlikely to explain the observed behavior. The decomposition of TOMCAT ozone time series and ERA5 geopotential height into the first two wavenumber components shows a clear correlation between the two variables in the middle stratosphere and demonstrates a weakening and a shift in the wavenumber‐1 planetary wave activity over the past two decades. Finally, the analysis of the polar vortex position and strength points to a decadal oscillation with a reversal pattern at the beginning of the century. The same is found in the ozone trend asymmetry. This further stresses the link between changes in the polar vortex position and the identified ozone trend pattern.

Revised estimates of NO2 reductions during the COVID-19 lockdowns using updated TROPOMI NO2 retrievals and model simulations

The TROPOspheric Monitoring Instrument (TROPOMI) observed unprecedented declines in NO2 vertical column densities (VCD) over the world's most densely populated cities during the 2020 COVID-19 lockdowns. These favorable changes in NO2 air quality were correlated with sharp reductions in traffic volume and economic activity during the lockdowns. In this comprehensive global study, we provide revised estimates of the declines in anthropogenic emissions for 36 megacities using a novel methodology for disentangling the anthropogenic emissions from the meteorological transport and natural variability. We further quantify the uncertainty associated with changes in the a priori profile shape information during the lockdowns due to reduced emissions. Satellite NO2 retrieval techniques calculate an air mass factor that requires a priori NO2 profile shape information representative of the local atmosphere. This information, which is typically obtained from a chemical transport model (CTM), was not available for the early studies. This study also accounts for the satellite sampling errors resulting from the selective sampling of non-cloudy scenes during the study period. For our analysis, we used CTM simulations that were generated with and without COVID-impacted emissions. We perform retrievals of tropospheric NO2 columns with the NASA NO2 algorithm, and then use observed and simulated data to disentangle the meteorological transport from the contribution due anthropogenic emissions. We found that the meteorological transport was most significant source of variability ranging between −35% and 22% of the change total tropospheric VCD. We also find that not accounting for changes in the a priori NO2 profile shape information during the lockdowns resulted in systematic retrieval errors that were up to 12% of the estimated decline, and the elimination of cloud contaminated scenes resulted in sampling errors that in general ranged between varied ±15%.

North Korean CO emissions reconstruction using DMZ ground observations, TROPOMI space-borne data, and the CMAQ air quality model

Emission uncertainty in North Korea can act as an obstacle when developing air pollution management plans in the country and neighboring countries when the transboundary transport of air pollutants is considered. This study introduces a novel approach for adjusting and reallocating North Korean CO emissions, aiming to complement the limited observational and emissions data on the country's air pollutants. We utilized ground observations from demilitarized zone (DMZ) and vertical column density (VCD) data from a TROPOspheric Monitoring Instrument (TROPOMI), which were combined with the Community Multi-Scale Air Quality (CMAQ) chemistry transport model simulations. The Clean Air Support System (CAPSS) and Satellite Integrated Joint Monitoring of Air Quality (SIJAQ) emissions inventories served as the basis for our initial simulations. A two-step procedure was proposed to adjust both the emission intensity and the spatial distribution of emissions. First, air quality simulations were conducted to explore model sensitivity to changes in North Korean CO emissions with respect to ground concentrations. DMZ observations then constrained these simulations to estimate corresponding emission intensity. Second, the spatial structure of North Korean CO emission sources was reconstructed with the help of TROPOMI CO VCD distributions. Our two-step hybrid method outperformed individual emissions adjustment and spatial reallocation based solely on surface or satellite observations. Validation using ground observations from the Chinese Dandong site near the China-North Korea border revealed significantly improved model simulations when applying the updated CO emissions. The adjusted CO emissions were 10.9 times higher than those derived from the bottom-up emissions used in this study, highlighting the lack of information on North Korean pollutants and emission sources. This approach offers an efficient and practical solution for identifying potential missing emission sources when there is limited on-site information about air quality on emissions.

Underappreciated Emission Spikes From Power Plants During Heatwaves Observed From Space: Case Studies in India and China

AbstractThe frequency, intensity, and duration of extreme heatwaves are projected to increase in the global context of climate change. However, evidence of how anthropogenic emissions respond to heatwaves and further impact air quality remains elusive. Here, we use satellite remote sensing measurements alongside chemical transport model simulations to reveal abrupt variations in primary and secondary air pollutants introduced by extreme heatwaves. We highlight evidence from China and India, where satellite sulfur dioxide (SO2) and nitrogen dioxide (NO2) columns over thermal power plants enhance consistently responding to heatwaves. We attribute such spiked emissions to soaring electricity use and demonstrate that bottom‐up inventories underestimate the emissions from the power sector by 34.9% for the selected case. Elevated emissions facilitate fine particulate matter (PM2.5) and ozone (O3) formation over thermal power plants in an inhomogeneous manner, due to the combined effect of atmospheric oxidizing capacity, thermal decomposition of peroxyacetyl nitrate, planetary boundary layer rise, and air stagnation. Our results underscore the emerging challenge of pollution control attributable to the increasing climate penalty and the necessity of targeted control strategies and alternative energy sources during heatwaves.

DIRECT AND INDIRECT CAUSAL EFFECTS OF AIR POLLUTANTS ON ALZHEIMER’S DISEASE RISK AND DISPARITIES

Abstract Ambient air contaminants have been associated with higher risk of Alzheimer’s disease (AD), related dementia, and cognitive impairment; however, mechanisms that underlay these effects remain unclear. Pre-existing arterial hypertension, diabetes mellitus, cerebrovascular disease, and renal disease have a strong impact on AD risk and disparities. These diseases, in turn, are associated with exposure to air contaminants, including particulate matter (PM2.5). We applied causal mediation analysis in the formulation of VanderWeele which provides causal estimates of the direct and indirect (through the effects on pre-existing diseases) effects of PM2.5 exposure on the risk of AD. We used Administrative Health Insurance Claims from 5%-Medicare (N=6,042,239; 1991-2020) to identify the date of onset for AD and risk related diseases such as arterial hypertension, diabetes, cerebrovascular, and kidney diseases that were considered mediators in these analyses. Information on ambient PM2.5 at the zip code level were derived from the Socioeconomic Data and Applications Center (SEDAC) that incorporates air monitoring data, satellite aerosol optical depth, meteorological conditions, chemical transport model simulations, and land-use variables. The estimates supported the hypotheses on the linear dependence of the dose-response function with higher effects for Males vs. Females, White vs. Black subpopulations, and stroke-belt states vs. other U.S. regions. We found that the contributions of indirect effects were stronger for younger older adults and reached up to 13% for cerebrovascular disease, 10% for arterial hypertension, 5% for diabetes, and 4% for chronic kidney disease. Analysis in subpopulations demonstrated health disparities in the effects of PM2.5 on AD risk.

A decadal atmospheric ammonia reanalysis product in China

Atmospheric ammonia has great environmental implications due to its important role in ecosystem and nitrogen cycle, as well as contribution to formation of secondary particles. China is recognized as a hotspot of NH3 pollution owing to agricultural and livestock intensification. In the quest to achieve a comprehensive understanding of atmospheric ammonia load and to quantify its environmental impacts in China, relying solely either on existing measurements or on model simulations falls short. Their limitations, either in spatial coverage and integrity or in data quality, fails to meet the needs. Available reanalysis products exhibit a marked deficiency in ammonia data. We therefore aim to propose an integrated ammonia reanalysis product in China, adeptly melding satellite observations from the Infrared Atmospheric Sounding Interferometer (IASI) NH3 retrievals with chemical transport model simulation, capitalizing on the robust Ensemble Kalman Filter (EnKF) data assimilation methodology. The product is validated in high quality via the comparison against independent measurements from ground monitoring stations. Spanning a decade from 2013 to 2022, our reanalysis uncovers not just the spatial intricacies of NH3 concentrations but also their temporal dynamics. Our findings pinpointed the spatial disparities in atmospheric ammonia intensities, highlighting regional hotspots in the NCP, SCB, and Northeast China, and identified annual and seasonal patterns. Our research provides crucial insights for shaping future NH3 pollution prevention and control strategies in China.

Contrasting changes in ozone during 2019–2021 between eastern and the other regions of China attributed to anthropogenic emissions and meteorological conditions

Ozone pollution is one of the most severe air quality issues in China that poses a serious threat to human health and ecosystems. During 2019–2021, the maximum daily 8-h average ozone concentrations in eastern China (110–122.5°E, 26–42°N) and the rest of China (ROC) show different decreasing patterns, with ozone concentrations in eastern China decreasing by 14.9 μg/m3, which is much larger than 4.8 μg/m3 in ROC. Here, based on two independent methods, the atmospheric chemical transport model (GEOS-Chem) simulations and the machine learning (ML) model (LightGBM) predictions, the reasons for the differences in ozone changes between eastern China and ROC during the warm season (April to September) are investigated. According to the GEOS-Chem (LightGBM) results, changes in the meteorological conditions contributed to an ozone decrease by 7.3 (6.8) μg/m3 in eastern China due to decreased chemical production and an ozone decrease by 6.8 (7.0) μg/m3 in ROC attributed to the weakened horizontal and vertical advection. With the influence of meteorological factors excluded, the observations show that changes in anthropogenic emissions resulted in an ozone decrease by 7.6 (8.1) μg/m3 in eastern China and an ozone increase by 2.0 (2.2) μg/m3 in ROC, which is primarily induced by the changes in NOx emissions. The surface measurements and satellite retrievals also indicate that the reduction in NOx emissions in ROC is less efficient than that in the more developed eastern China, leading to contrasting changes in ozone concentrations between eastern China and ROC during 2019–2021. Our results highlight the critical need to reduce ozone precursor emissions in the rest regions of China apart from eastern China.

Effects of simulated secondary organic aerosol water on PM1 levels and composition over the US

Abstract. Water is a key component of atmospheric aerosol, affecting many aerosol processes including gas-to-particle partitioning of semi-volatile compounds. Water related to secondary organic aerosol (SOAW) is often neglected in atmospheric chemical transport models and is not considered in gas-to-particle partitioning calculations for inorganic species. We use a new inorganic aerosol thermodynamics model, ISORROPIA-lite, which considers the effects of SOAW, to perform chemical transport model simulations for 1 year over the continental United States to quantify its effects on aerosol mass concentration and composition. SOAW can increase average fine aerosol water levels by up to a factor of 2 when secondary organic aerosol (SOA) is a major PM1 component. This is often the case in the south-eastern US, where SOA concentrations are higher. Although the annual average impact of this added water on total dry PM1 concentrations due to increased partitioning of nitrate and ammonium is small (up to 0.1 µg m−3), total dry PM1 increases of up to 2 µg m−3 (with nitrate levels increases of up to 200 %) can occur when RH levels and PM1 concentrations are high.

Quantifying stratospheric ozone trends over 1984–2020: a comparison of ordinary and regularized multivariate regression models

Abstract. Accurate quantification of long-term trends in stratospheric ozone can be challenging due to their sensitivity to natural variability, the quality of the observational datasets, and non-linear changes in forcing processes as well as the statistical methodologies. Multivariate linear regression (MLR) is the most commonly used tool for ozone trend analysis; however, the complex coupling in many atmospheric processes can make it prone to the issue of over-fitting when using the conventional ordinary-least-squares (OLS) approach. To overcome this issue, here we adopt a regularized (ridge) regression method to estimate ozone trends and quantify the influence of individual processes. We use the Stratospheric Water and OzOne Satellite Homogenized (SWOOSH) merged dataset (v2.7) to derive stratospheric ozone profile trends for the period 1984–2020. Besides SWOOSH, we also analyse a machine-learning-based satellite-corrected gap-free global stratospheric ozone profile dataset from a chemical transport model (ML-TOMCAT) and output from a chemical transport model (TOMCAT) simulation forced with European Centre for Medium-Range Weather Forecasts (ECMWF) ERA5 reanalysis. For 1984–1997, we observe smaller negative trends in the SWOOSH stratospheric ozone profile using ridge regression compared to OLS. Except for the tropical lower stratosphere, the largest differences arise in the mid-latitude lowermost stratosphere (>4 % per decade difference at 100 hPa). From 1998 and the onset of ozone recovery in the upper stratosphere, the positive trends estimated using the ridge regression model (∼1 % per decade near 2 hPa) are smaller than those using OLS (∼2 % per decade). In the lower stratosphere, post-1998 negative trends with large uncertainties are observed and ridge-based trend estimates are somewhat smaller and less variable in magnitude compared to the OLS regression. Aside from the tropical lower stratosphere, the largest difference is around 2 % per decade at 100 hPa (with ∼3 % per decade uncertainties for individual trends) in northern mid-latitudes. For both time periods the SWOOSH data produce large negative trends in the tropical lower stratosphere with a correspondingly large difference between the two trend methods. In both cases the ridge method produces a smaller trend. The regression coefficients from both OLS and ridge models, which represent ozone variations associated with natural processes (e.g. the quasi-biennial oscillation, solar variability, El Niño–Southern Oscillation, Arctic Oscillation, Antarctic Oscillation, and Eliassen–Palm flux), highlight the dominance of dynamical processes in controlling lower-stratospheric ozone concentrations. Ridge regression generally yields smaller regression coefficients due to correlated explanatory variables, and care must be exercised when comparing fit coefficients and their statistical significance across different regression methods. Comparing the ML-TOMCAT-based trend estimates with the ERA5-forced model simulation, we find ML-TOMCAT shows significant improvements with much better consistency with the SWOOSH dataset, despite the ML-TOMCAT training period overlapping with SWOOSH only for the Microwave Limb Sounder (MLS) measurement period. The largest inconsistencies with respect to SWOOSH-based trends post-1998 appear in the lower stratosphere where the ERA5-forced model simulation shows positive trends for both the tropics and the mid-latitudes. The large differences between satellite-based data and the ERA5-forced model simulation confirm significant uncertainties in ozone trend estimates, especially in the lower stratosphere, underscoring the need for caution when interpreting results obtained with different regression methods and datasets.

Unveiling the underestimated direct emissions of nitrous acid (HONO)

Gaseous nitrous acid (HONO) is a critical source of hydroxyl radicals (OH) in the troposphere. While both direct and secondary sources contribute to atmospheric HONO, direct emissions have traditionally been considered minor contributors. In this study, we developed δ15N and δ18O isotopic fingerprints to identify six direct HONO emission sources and conducted a 1-y case study on the isotopic composition of atmospheric HONO at rural and urban sites. Interestingly, we identified that livestock farming is a previously overlooked direct source of HONO and determined its HONO to ammonia (NH3) emission ratio. Additionally, our results revealed that spatial and temporal variations in atmospheric HONO isotopic composition can be partially attributed to direct emissions. Through a detailed HONO budget analysis incorporating agricultural sources, we found that direct HONO emissions accounted for 39~45% of HONO production in rural areas across different seasons. The findings were further confirmed by chemistry transport model simulations, highlighting the significance of direct HONO emissions and their impact on air quality in the North China Plain. These findings provide compelling evidence that direct HONO emissions play a more substantial role in contributing to atmospheric HONO than previously believed. Moreover, the δ15N and δ18O isotopic fingerprints developed in this study may serve as a valuable tool for further research on the atmospheric chemistry of reactive nitrogen gases.

Soil Emissions of Reactive Nitrogen Accelerate Summertime Surface Ozone Increases in the North China Plain.

Summertime surface ozone in China has been increasing since 2013 despite the policy-driven reduction in fuel combustion emissions of nitrogen oxides (NOx). Here we examine the role of soil reactive nitrogen (Nr, including NOx and nitrous acid (HONO)) emissions in the 2013-2019 ozone increase over the North China Plain (NCP), using GEOS-Chem chemical transport model simulations. We update soil NOx emissions and add soil HONO emissions in GEOS-Chem based on observation-constrained parametrization schemes. The model estimates significant daily maximum 8 h average (MDA8) ozone enhancement from soil Nr emissions of 8.0 ppbv over the NCP and 5.5 ppbv over China in June-July 2019. We identify a strong competing effect between combustion and soil Nr sources on ozone production in the NCP region. We find that soil Nr emissions accelerate the 2013-2019 June-July ozone increase over the NCP by 3.0 ppbv. The increase in soil Nr ozone contribution, however, is not primarily driven by weather-induced increases in soil Nr emissions, but by the concurrent decreases in fuel combustion NOx emissions, which enhance ozone production efficiency from soil by pushing ozone production toward a more NOx-sensitive regime. Our results reveal an important indirect effect from fuel combustion NOx emission reduction on ozone trends by increasing ozone production from soil Nr emissions, highlighting the necessity to consider the interaction between anthropogenic and biogenic sources in ozone mitigation in the North China Plain.

Estimating surface-level nitrogen dioxide concentrations from Sentinel-5P/TROPOMI observations in Finland

In recent decades, satellite instruments have been providing observations of air pollutants such as nitrogen dioxide (NO2) with global coverage. Since late 2018, the TROPOspheric Monitoring Instrument (TROPOMI) on-board the Copernicus Sentinel-5 Precursor satellite has produced NO2 vertical column densities (VCDs) with the best spatial resolution (currently 5.5 × 3.5km2 at nadir). In this paper, we test and adapt two previously published methods to estimate surface-level NO2 concentrations from TROPOMI VCD retrievals in the specific conditions of Finland. Satellite-based estimates show good correlation with co-located surface NO2 measurements from the Finnish AQ network, although not accounting for the level of NO2 mixing within the boundary layer leads to underestimation. We also use a linear relation between in situ measurements and surface-level estimates to correct for the observed negative bias in the estimates. Finally, we use chemical transport model simulations to estimate the ratio of the annual mean surface concentrations to the values sampled according to TROPOMI observation times, and use it to correct our surface-level NO2 estimates for compatibility with annual limit values defined in AQ legislation.Overall, the results provide new information to complement traditional ground-based AQ measurements, especially over areas where the surface AQ networks are sparse, and to support national environmental authorities in air quality assessment and reporting.

Development of a recurrent spatiotemporal deep-learning method coupled with data fusion for correction of hourly ozone forecasts

Ambient ozone (O3) predictions can be very challenging mainly due to the highly nonlinear photochemistry among its precursors, and meteorological conditions and regional transport can further complicate the O3 formation processes. The emission-based chemical transport models (CTM) are broadly used to predict O3 formation, but they may deviate from observations due to input uncertainties such as emissions and meteorological data, in addition to the treatment of O3 nonlinear chemistry. In this study, an innovative recurrent spatiotemporal deep-learning (RSDL) method with model-monitor coupled convolutional recurrent neural networks (ConvRNN) has been developed to improve O3 predictions of CTM. The RSDL method was first used to build the ConvRNN within a 24-h scale to characterize the spatiotemporal relationships between the monitored O3 data and CTM simulations, and then incorporated the recurrent pattern to achieve 72-h multi-site forecasts based on a pilot study over the Pearl River Delta (PRD) region of China. The results showed that the RSDL method predicted O3 with high accuracy over this case study, with an increase of 27.54% in the correlation coefficient (R) average for all sites as well as an increase in R of 0.14–0.21 for all cities compared to CTM. Moreover, the regional distribution of CTM was further improved by the RSDL predictions with the data fusion technique, which greatly reduced the underpredictions of O3 concentrations, particularly in high O3-level areas (concentrations >160 μg/m3), with a 33.55% reduction in the mean absolute error (MAE).

High-resolution downscaling of source resolved PM2.5 predictions using machine learning models

Accurate predictions of source resolved atmospheric PM2.5 concentrations at high resolutions using chemical transport models (CTMs) require expensive CTM simulations and development of high-resolution emissions inventories. We use multiple machine learning (ML) approaches to downscale coarse-resolution (36 × 36 km2) CTM predictions to 1 × 1 km2 spatial resolution. ML predictions include concentrations of the major chemical components of PM2.5 and the contributions of its major emissions sources. Inputs for the ML models include 36 × 36 km2 source resolved CTM predicted concentrations of all PM2.5 components, meteorological data, and several land-use (LU) variables. The output of our ML models is the 1 × 1 km2 source-resolved concentrations of all major PM2.5 components in southwestern Pennsylvania (5184 km2 domain) during February and July 2017. Models were trained and validated using 1 × 1 km2 resolution source- and species-resolved CTM predictions of PM2.5 from recent complementary studies. The best overall performance was found using a random forest (RF) model, where species and source resolved PM2.5 concentrations were reproduced with low normalized mean bias (|NMB| < 0.01). The downscaling model captures the spatial distribution of PM2.5 both by component and source, with some discrepancies when predicting the plumes of large point sources that have long-range impacts. In a test of generalizability to unknown domains, the model differentiates well between areas that are primarily urban, rural, or industrial but faces challenges with the reproduction of the effects of large point sources of PM2.5 when entire quadrants are removed from the training data. The results represent a proof of concept for downscaling low-resolution CTM predictions using native high-resolution CTM predictions in training.