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Further long-term investments in high-quality, research-driven, fit-for-purpose observations of atmospheric composition are needed globally to meet urgent societal needs related to weather, climate, air quality, and other environmental issues. Challenges include maintaining current observing systems in the face of eroding budgets for long-term monitoring and filling the geographical gaps for key constituents needed for sound services and policies. The observing systems can be bolstered through science-for-services applications, by embracing interoperable observation systems and standardized metadata, and ensuring that the data are findable, accessible, interoperable, and reusable. There is an urgent need to move from opportunities-driven one-component observations to more systematic, planned multifunctional infrastructure, where the observational data flow is coupled with Earth system models to serve both operational and research purposes. This approach fosters a community where user experience feeds back into the research components and where mature research results are translated into operational applications. This will lead to faster exploration and exploitation of atmospheric composition information and more impactful applications for science and society. We discuss here the urgent need to (i) achieve global coverage, (ii) harmonize infrastructure operations, (iii) establish focused policies, and (iv) strengthen coordination of atmospheric composition infrastructure.

A new open biomass burning inventory is presented that relies on the fire radiative power data from the Visible Infrared Imaging Radiometer Suite (VIIRS) on board the Suomi NPP satellite. This VIIRS-based Fire Emission Inventory (VFEI) provides emission data from early 2012 to 2019 for more than 40 species of gases and aerosols at spatial resolutions of around 500 m. We found that VFEI produces similar results when compared to other major inventories in many regions of the world. Additionally, we conducted regional simulations using VFEI with the Weather Research and Forecasting (WRF) model with chemistry (WRF-Chem) for Southern Africa (September 2016) and North America (July–August 2019). We compared aerosol optical depth (AOD) from the model against two observational datasets: the MODIS Multi-Angle Implementation of Atmospheric Correction (MAIAC) product and AErosol RObotic NETwork (AERONET) stations. Results showed good agreement between both simulations and the datasets, with mean AOD biases of around +0.03 for Southern Africa and −0.01 for North America. Both simulations were not only able to reproduce the AOD magnitudes accurately, but also the inter-diurnal variations of smoke concentration. In addition, we made use of the airborne data from the ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES; Southern Africa) and the Fire Influence on Regional to Global Environments Experiment and Air Quality (FIREX-AQ; North America) campaigns to evaluate the simulations. In Southern Africa, results showed correlations higher than 0.77 when comparing carbon monoxide and black carbon. In North America, correlations were lower and biases higher. However, this is because the model was not able to reproduce the timing, shape, and location of individual plumes over complex terrain (Rocky Mountains) during the FIREX-AQ campaign period.

Concentrations of ambient particulate matter (such as PM2.5 and PM10) have come to represent a serious environmental problem worldwide, causing many deaths and economic losses. Because of the detrimental effects of PM2.5 on human health, many countries and international organizations have developed and operated regional and global short-term PM2.5 prediction systems. The short-term predictability of PM2.5 (and PM10) is determined by two main factors: the performance of the air quality model and the accuracy of the initial states. While specifically focusing on the latter factor, this study attempts to demonstrate how information from ‘classical’ ground observation networks, a ‘state-of-the-art’ geostationary (GEO) satellite sensor, and an advanced air quality modeling system can be synergistically combined to improve short-term PM2.5 predictability over South Korea. Such a synergistic combination of information can effectively overcome the major obstacle of scarcity of information, which frequently occurs in PM2.5 prediction systems using low Earth orbit (LEO) satellite-borne observations. This study first presents that the scarcity of information is mainly associated with cloud masking, sun-glint effect, and ill-location of satellite-borne data, and it then demonstrates that an advanced air quality modeling system equipped with synergistically-combined information can achieve substantially improved performances, producing enhancements of approximately 10%, 17%, 49%, and 19% in the predictability of PM2.5 over South Korea in terms of IOA (index of agreement), R (correlation coefficient), MB (mean biases), and HR (hit rate), respectively, compared to PM2.5 prediction systems using only LEO satellite-derived observations.

The unprecedented lockdown of human activities during the COVID-19 pandemic have significantly influenced the social life in China. However, understanding of the impact of this unique event on the emissions of different species is still insufficient, prohibiting the proper assessment of the environmental impacts of COVID-19 restrictions. Here we developed a multi-air pollutant inversion system to simultaneously estimate the emissions of NOx, SO2, CO, PM2.5 and PM10 in China during COVID-19 restrictions with high temporal (daily) and horizontal (15km) resolutions. Subsequently, contributions of emission changes versus meteorology variations during COVID-19 lockdown were separated and quantified. The results demonstrated that the inversion system effectively reproduced the actual emission variations of multi-air pollutants in China during different periods of COVID-19 lockdown, which indicate that the lockdown is largely a nationwide road traffic control measurement with NOx emissions decreased substantially by ~40%. However, emissions of other air pollutants were found only decreased by ~10%, both because power generation and heavy industrial processes were not halted during lockdown, and residential activities may actually have increased due to the stay-at-home orders. Consequently, although obvious reductions of PM2.5 concentrations occurred over North China Plain (NCP) during lockdown period, the emission change only accounted for 8.6% of PM2.5 reductions, and even led to substantial increases of O3. The meteorological variation instead dominated the changes in PM2.5 concentrations over NCP, which contributed 90% of the PM2.5 reductions over most parts of NCP region. Meanwhile, our results also suggest that the local stagnant meteorological conditions together with inefficient reductions in PM2.5 emissions were the main drivers of the unexpected COVID-19 haze in Beijing. These results highlighted that traffic control as a separate pollution control measure has limited effects on the coordinated control of O3 and PM2.5 concentrations under current complex air pollution conditions in China. More comprehensive and balanced regulations for multiple precursors from different sectors are required to address O3 and PM2.5 pollution in China.

The southeastern Atlantic is home to an expansive smoke aerosol plume overlying a large cloud deck for approximately a third of the year. The aerosol plume is mainly attributed to the extensive biomass burning activities that occur in southern Africa. Current Earth system models (ESMs) reveal significant differences in their estimates of regional aerosol radiative effects over this region. Such large differences partially stem from uncertainties in the vertical distribution of aerosols in the troposphere. These uncertainties translate into different aerosol optical depths (AODs) in the planetary boundary layer (PBL) and the free troposphere (FT). This study examines differences of AOD fraction in the FT and AOD differences among ESMs (WRF-CAM5, WRF-FINN, GEOS-Chem, EAM-E3SM, ALADIN, GEOS-FP, and MERRA-2) and aircraft-based measurements from the NASA ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) field campaign. Models frequently define the PBL as the well-mixed surface-based layer, but this definition misses the upper parts of decoupled PBLs, in which most low-level clouds occur. To account for the presence of decoupled boundary layers in the models, the height of maximum vertical gradient of specific humidity profiles from each model is used to define PBL heights. Results indicate that the monthly mean contribution of AOD in the FT to the total-column AOD ranges from 44 % to 74 % in September 2016 and from 54 % to 71 % in August 2017 within the region bounded by 25∘ S–0∘ N–S and 15∘ W–15∘ E (excluding land) among the ESMs. ALADIN and GEOS-Chem show similar aerosol plume patterns to a derived above-cloud aerosol product from the Moderate Resolution Imaging Spectroradiometer (MODIS) during September 2016, but none of the models show a similar above-cloud plume pattern to MODIS in August 2017. Using the second-generation High Spectral Resolution Lidar (HSRL-2) to derive an aircraft-based constraint on the AOD and the fractional AOD, we found that WRF-CAM5 produces 40 % less AOD than those from the HSRL-2 measurements, but it performs well at separating AOD fraction between the FT and the PBL. AOD fractions in the FT for GEOS-Chem and EAM-E3SM are, respectively, 10 % and 15 % lower than the AOD fractions from the HSRL-2. Their similar mean AODs reflect a cancellation of high and low AOD biases. Compared with aircraft-based observations, GEOS-FP, MERRA-2, and ALADIN produce 24 %–36 % less AOD and tend to misplace more aerosols in the PBL. The models generally underestimate AODs for measured AODs that are above 0.8, indicating their limitations at reproducing high AODs. The differences in the absolute AOD, FT AOD, and the vertical apportioning of AOD in different models highlight the need to continue improving the accuracy of modeled AOD distributions. These differences affect the sign and magnitude of the net aerosol radiative forcing, especially when aerosols are in contact with clouds.

Vehicle emissions are regarded as a primary contributor to air pollution and related adverse health impacts. Heavy traffic congestion increases traffic flow and thus produces more O3 precursor emissions, leading to more adverse air quality issues. Although the development of a vehicle emission inventory has received great concern and continuous efforts, limitations still exist. For example, real-time diurnal variations and increases in emission rates due to traffic congestion are not well understood. In this study, we developed a new temporal allocation approach in transportation emissions to investigate the impact on air quality and health burden due to traffic congestion in China in 2020. Both real-time congestion-level data and emission correction factors were considered in the approach. Results show that traffic congestion aggravates air pollution and health burden across China, especially in the urban clusters such as the North China Plain and Sichuan Basin. In these regions, the average annual increases in fine particulate matter (PM2.5) and ozone (O3) could be up to 3.5 µg m−3 and 1.1 ppb, respectively. The excess PM2.5 and O3 attributed to the traffic congestion also induce an additional 20 000 and 5000 premature deaths in China, respectively. In major cities, the increased rate of premature mortality caused by traffic congestion may reach 17.5 %. Therefore, more effective and comprehensive vehicle emission control policies or better planning of the road network should be established to reduce traffic congestion and improve air quality in China.

The Lake Michigan Ozone Study 2017 (LMOS 2017) was a collaborative multiagency field study targeting ozone chemistry, meteorology, and air quality observations in the southern Lake Michigan area. The primary objective of LMOS 2017 was to provide measurements to improve air quality modeling of the complex meteorological and chemical environment in the region. LMOS 2017 science questions included spatiotemporal assessment of nitrogen oxides (NOx = NO + NO2) and volatile organic compounds (VOC) emission sources and their influence on ozone episodes; the role of lake breezes; contribution of new remote sensing tools such as GeoTASO, Pandora, and TEMPO to air quality management; and evaluation of photochemical grid models. The observing strategy included GeoTASO on board the NASA UC-12 aircraft capturing NO2 and formaldehyde columns, an in situ profiling aircraft, two ground-based coastal enhanced monitoring locations, continuous NO2 columns from coastal Pandora instruments, and an instrumented research vessel. Local photochemical ozone production was observed on 2 June, 9–12 June, and 14–16 June, providing insights on the processes relevant to state and federal air quality management. The LMOS 2017 aircraft mapped significant spatial and temporal variation of NO2 emissions as well as polluted layers with rapid ozone formation occurring in a shallow layer near the Lake Michigan surface. Meteorological characteristics of the lake breeze were observed in detail and measurements of ozone, NOx, nitric acid, hydrogen peroxide, VOC, oxygenated VOC (OVOC), and fine particulate matter (PM2.5) composition were conducted. This article summarizes the study design, directs readers to the campaign data repository, and presents a summary of findings.

This study evaluates the impact of satellite soil moisture (SM) data assimilation (DA) on regional weather and ozone (O3) modeling over the southeastern US during the summer. Satellite SM data are assimilated into the Noah land surface model using an ensemble Kalman filter approach within National Aeronautics and Space Administration's Land Information System framework, which is semicoupled with the Weather Research and Forecasting model with online Chemistry (WRF-Chem; standard version 3.9.1.1). The DA impacts on the model performance of SM, weather states, and energy fluxes show strong spatiotemporal variability. Dense vegetation and water use from human activities unaccounted for in the modeling system are among the factors impacting the effectiveness of the DA. The daytime surface O3 responses to the DA can largely be explained by the temperature-driven changes in biogenic emissions of volatile organic compounds and soil nitric oxide, chemical reaction rates, and dry deposition velocities. On a near-biweekly timescale, the DA modified the mean daytime and daily maximum 8 h average surface O3 by up to 2–3 ppbv, with the maximum impacts occurring in areas where daytime surface air temperature most strongly (i.e., by ∼2 K) responded to the DA. The DA impacted WRF-Chem upper tropospheric O3 (e.g., for its daytime-mean, by up to 1–1.5 ppbv) partially via altering the transport of O3 and its precursors from other places as well as in situ chemical production of O3 from lightning and other emissions. Case studies during airborne field campaigns suggest that the DA improved the model treatment of convective transport and/or lightning production. In the cases that the DA improved the modeled SM, weather fields, and some O3-related processes, its influences on the model's O3 performance at various altitudes are not always as desirable. This is in part due to the uncertainty in the model's key chemical inputs, such as anthropogenic emissions, and the model representation of stratosphere–troposphere exchanges. This can also be attributable to shortcomings in model parameterizations (e.g., chemical mechanism, natural emission, photolysis and deposition schemes), including those related to representing water availability impacts. This study also shows that the WRF-Chem upper tropospheric O3 response to the DA has comparable magnitudes with its response to the estimated US anthropogenic emission changes within 2 years. As reductions in anthropogenic emissions in North America would benefit the mitigation of O3 pollution in its downwind regions, this analysis highlights the important role of SM in quantifying air pollutants' source–receptor relationships between the US and its downwind areas. It also emphasizes that using up-to-date anthropogenic emissions is necessary for accurately assessing the DA impacts on the model performance of O3 and other pollutants over a broad region. This work will be followed by a Noah-Multiparameterization (with dynamic vegetation)-based study over the southeastern US, in which selected processes including photosynthesis and O3 dry deposition will be the foci.

Monitoring and modeling/predicting air pollution are crucial to understanding the links between emissions and air pollution levels, to supporting air quality management, and to reducing human exposure. Yet, current monitoring networks and modeling capabilities are unfortunately inadequate to understand the physical and chemical processes above ground and to support attribution of sources. We highlight the need for the development of an international stereoscopic monitoring strategy that can depict three-dimensional (3D) distribution of atmospheric composition to reduce the uncertainties and to advance diagnostic understanding and prediction of air pollution. There are three reasons for the implementation of stereoscopic monitoring: 1) current observation networks provide only partial view of air pollution, and this can lead to misleading air quality management actions; 2) satellite retrievals of air pollutants are widely used in air pollution studies, but too often users do not acknowledge that they have large uncertainties, which can be reduced with measurements of vertical profiles; and 3) air quality modeling and forecasting require 3D observational constraints. We call on researchers and policymakers to establish stereoscopic monitoring networks and share monitoring data to better characterize the formation of air pollution, optimize air quality management, and protect human health. Future directions for advancing monitoring and modeling/predicting air pollution are also discussed.

The southeast Atlantic is home to an expansive smoke aerosol plume overlying a large cloud deck for approximately a third of the year. The aerosol plume is mainly attributed to the extensive biomass burning activity that occurs in southern Africa. Current Earth system models (ESMs) reveal significant differences in their estimates of regional aerosol radiative effects over this region. Such large differences partially stem from uncertainties in the vertical distribution of aerosols in the troposphere. These uncertainties translate into different aerosol optical depths (AOD) in the planetary boundary layer (PBL) and the free troposphere (FT). This study examines differences of AOD fraction in the FT and AOD differences among ESMs (WRF-CAM5, WRF-FINN, GEOS-Chem, EAM-E3SM, ALADIN, GEOS-FP, and MERRA-2) and aircraft-based measurements from the NASA ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) field campaign. Models frequently define the PBL as the well-mixed surface-based layer, but this definition misses the upper parts of decoupled PBLs, in which most low-level clouds occur. To account for the presence of decoupled boundary layers in the models, the height of maximum vertical gradient of specific humidity profiles from each model is used to define PBL heights. Results indicate that the monthly mean contribution of AOD in the FT to the total-column AOD ranges from 44 % to 74 % in September 2016 and from 54 % to 71 % in August 2017 within the region bounded by 25°S–0° and 15°W–15°E (excluding land) among the ESMs. Using the second-generation High Spectral Resolution Lidar (HSRL-2) to derive an aircraft-based constraint on the AOD and the fractional AOD, we found that WRF-CAM5 produces 40 % less AOD than those from the HSRL-2 measurements, but it performs well at separating AOD fraction between the FT and the PBL. AOD fractions in the FT for GEOS-Chem and EAM-E3SM are, respectively, 10 % and 15 % lower than the AOD fractions from the HSRL-2 and their similarities in the mean AODs are the result of cancellation of high and low AOD biases. GEOS-FP, MERRA-2, and ALADIN produce 24 %–36 % less AOD and tend to misplace more aerosols in the PBL compared to aircraft-based observations. The models generally underestimate AODs for measured AODs that are above 0.8, indicating their limitations at reproducing high AODs. The differences in the absolute AOD, FT AOD, and the vertical apportioning of AOD in different models highlight the need to continue improving the accuracy of modeled AOD distributions. These differences affect the sign and magnitude of the net aerosol radiative forcing, especially when aerosols are in contact with clouds.

Limitations in the current capability of monitoring PM2.5 adversely impact air quality management and health risk assessment of PM2.5 exposure. Commonly, ground-based monitoring networks are established to measure the PM2.5 concentrations in highly populated regions and protected areas such as national parks, yet large gaps exist in spatial coverage. Satellite-derived aerosol optical properties serve to complement the missing spatial information of ground-based monitoring networks. However, such attempts are hampered under cloudy/hazy conditions or during nighttime. Here we strive to overcome the long-standing restriction that surface PM2.5 cannot be constrained with satellite remote sensing under cloudy/hazy conditions or during nighttime. We introduce a deep spatiotemporal neural network (ST-NN) and demonstrate that it can artfully fill these observational gaps. We use sensitivity analysis and visualization technology to open the neural network black box data model, and quantitatively discuss the potential impact of the input data on the target variables. This technique provides ground-level PM2.5 concentrations with high spatial resolution (0.01°) and 24-hour temporal coverage. Better constrained spatiotemporal distributions of PM2.5 concentrations will help improve health effects studies, atmospheric emission estimates, and predictions of air quality.

Urbanization took place rapidly over recent decades and is expected to continue in the future, producing a series of environmental issues, including heat stress. Cool roof and green roof strategies have been adopted in a number of megacities to mitigate urban heat and carbon emissions, yet China is lagging behind developed countries in the implementation. One reason is the lack of careful and thoughtful assessment of potential effects of roof strategies, including their influences on winter PM2.5. With numerical simulations in this study, we assess how cool and green roof strategies affect winter PM2.5 pollution in North China, and we find that adoptions of cool roofs tend to aggravate PM2.5 pollution in lightly polluted regions. When PM2.5 pollution worsens, the negative effects of cool roofs are likely to be diminished. Green roofs cause less enhancements of PM2.5 pollution as a result of inhibited evapotranspiration in winter. We demonstrate that the effects of roof strategies are regulated by pollution severity and conclude that green roofs with suppressed evapotranspiration and thus weaker penalty on winter PM2.5 pollution seem to be better choices given the current pollution severity level in China, especially for regions suitable for growth of broadleaf plants.

This study compares the performance of 12 regional chemical transport models (CTMs) from the third phase of the Model Inter-Comparison Study for Asia (MICS-Asia III) on simulating the particulate matter (PM) over East Asia (EA) in 2010. The participating models include the Weather Research and Forecasting model coupled with Community Multiscale Air Quality (WRF-CMAQ; v4.7.1 and v5.0.2), the Regional Atmospheric Modeling System coupled with CMAQ (RAMS-CMAQ; v4.7.1 and v5.0.2), the Weather Research and Forecasting model coupled with chemistry (WRF-Chem; v3.6.1 and v3.7.1), Goddard Earth Observing System coupled with chemistry (GEOS-Chem), a non-hydrostatic model coupled with chemistry (NHM-Chem), the Nested Air Quality Prediction Modeling System (NAQPMS) and the NASA-Unified WRF (NU-WRF). This study investigates three model processes as the possible reasons for different model performances on PM. (1) Models perform very differently in the gas–particle conversion of sulfur (S) and oxidized nitrogen (N). The model differences in sulfur oxidation ratio (50 %) are of the same magnitude as that in SO42- concentrations. The gas–particle conversion is one of the main reasons for different model performances on fine mode PM. (2) Models without dust emission modules can perform well on PM10 at non-dust-affected sites but largely underestimate (up to 50 %) the PM10 concentrations at dust sites. The implementation of dust emission modules in the models has largely improved the model accuracies at dust sites (reduce model bias to −20 %). However, both the magnitude and distribution of dust pollution are not fully captured. (3) The amounts of modeled depositions vary among models by 75 %, 39 %, 21 % and 38 % for S wet, S dry, N wet and N dry depositions, respectively. Large inter-model differences are found in the washout ratios of wet deposition (at most 170 % in India) and dry deposition velocities (generally 0.3–2 cm s−1 differences over inland regions).

A new open biomass burning inventory is presented that relies on the fire radiative power data from the Visible Infrared Imaging Radiometer Suite (VIIRS) onboard the Suomi NPP satellite. This VIIRS-based Fire Emission Inventory (VFEI) provides emission data from early 2012 to 2019 for more than 40 species of gases and aerosols at spatial resolutions of around 500 m. We found that VFEI produces similar results when compared to other major inventories in many regions of the world. Additionally, we conducted regional simulations using VFEI with the Weather Research and Forecasting (WRF) model with chemistry (WRF-Chem) for Southern Africa (September 2016) and North America (July–August 2019). We compared aerosol optical depth (AOD) from the model against two observational datasets: the MODIS Multi-Angle Implementation of Atmospheric Correction (MAIAC) product and AErosol RObotic NETwork (AERONET) stations. Results showed good agreement between both simulations and the datasets, with mean AOD biases of around +0.03 for Southern Africa and –0.01 for North America. Both simulations were not only able to reproduce accurately the AOD magnitudes, but also the inter-diurnal variations of smoke concentration. In addition, we made use of the airborne data from the ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES; Southern Africa) and the Fire Influence on Regional to Global Environments Experiment and Air Quality (FIREX-AQ; North America) campaigns to evaluate the simulations. In Southern Africa, results showed correlations higher than 0.77 when comparing carbon monoxide and black carbon. In North America, correlations were lower and biases higher. However, this is because the model was not able to reproduce the timing, shape, and location of individual plumes over complex terrain (Rocky Mountains) during the FIREX-AQ campaign period.

Unprecedented urbanization in China has led to serious urban heat island (UHI) issues, exerting intense heat stress on urban residents. Based on the observed temperature and PM2.5 concentrations in Beijing over 2016–2020, we find diverse influences of aerosol pollution on urban heat island intensity (UHII) under different circulations. When northerly winds are prevalent in urban Beijing, UHII tends to be much higher in both daytime and nighttime and it is less affected by aerosol concentrations. However, when southerly and westerly winds are dominant in rural Beijing, UHII is significantly reduced by aerosol pollution. Using coupled aerosol-radiation weather simulations, we demonstrate the underlying physical mechanism which is associated with local circulation and resulting spatial distribution of aerosols. Our results also highlight the role of black carbon in aggravating UHI, especially during nighttime. It could thus be targeted for cooperative management of heat islands and aerosol pollution.

Earth system and environmental impact studies need high quality and up-to-date estimates of atmospheric deposition. This study demonstrates the methodological benefits of multimodel ensemble and measurement-model fusion mapping approaches for atmospheric deposition focusing on 2010, a year for which several studies were conducted. Global model-only deposition assessment can be further improved by integrating new model-measurement techniques, including expanded capabilities of satellite observations of atmospheric composition. We identify research and implementation priorities for timely estimates of deposition globally as implemented by the World Meteorological Organization.

Severe wintertime PM2.5 pollution in Beijing has been receiving increasing worldwide attention, yet the decadal variations remain relatively unexplored. Combining field measurements and model simulations, we quantified the relative influences of anthropogenic emissions and meteorological conditions on PM2.5 concentrations in Beijing over the winters of 2002–2016. Between the winters of 2011 and 2016, stringent emission control measures resulted in a 21 % decrease in mean mass concentrations of PM2.5 in Beijing, with 7 fewer haze days per winter on average. Given the overestimation of PM2.5 by the model, the effectiveness of stringent emission control measures might have been slightly overstated. With fixed emissions, meteorological conditions over the study period would have led to an increase in haze in Beijing, but the strict emission control measures have suppressed the unfavorable influences of the recent climate. The unfavorable meteorological conditions are attributed to the weakening of the East Asia winter monsoon associated particularly with an increase in pressure associated with the Aleutian Low.