This study presents the results from the Tropospheric Chemistry Reanalysis version 2 (TCR-2) for the period 2005–2018 at 1.1^∘ horizontal resolution obtained from the assimilation of multiple updated satellite measurements of ozone, CO, NO₂, HNO₃, and SO₂ from the OMI, SCIAMACHY, GOME-2, TES, MLS, and MOPITT satellite instruments. The reanalysis calculation was conducted using a global chemical transport model MIROC-CHASER and an ensemble Kalman filter technique that optimizes both chemical concentrations of various species and emissions of several precursors, which was efficient for the correction of the entire tropospheric profile of various species and its year-to-year variations. Comparisons against independent aircraft, satellite, and ozonesonde observations demonstrate the quality of the reanalysis fields for numerous key species on regional and global scales, as well as for seasonal, yearly, and decadal scales, from the surface to the lower stratosphere. The multi-constituent data assimilation brought the model vertical profiles and interhemispheric gradient of OH closer to observational estimates, which was important in improving the description of the oxidation capacity of the atmosphere and thus vertical profiles of various species. The evaluation results demonstrate the capability of the chemical reanalysis to improve understanding of the processes controlling variations in atmospheric composition, including long-term changes in near-surface air quality and emissions. The estimated emissions can be employed for the elucidation of detailed distributions of the anthropogenic and biomass burning emissions of co-emitted species (NO_x, CO, SO₂) in all major regions, as well as their seasonal and decadal variabilities. The data sets are available at https://doi.org/10.25966/9qgv-fe81 (Miyazaki et al., 2019 a).

Efforts to stem the transmission of coronavirus disease 2019 (COVID-19) led to rapid, global ancillary reductions in air pollutant emissions. Here, we quantify the impact on tropospheric ozone using a multiconstituent chemical data assimilation system. Anthropogenic NO_x emissions dropped by at least 15% globally and 18 to 25% regionally in April and May 2020, which decreased free tropospheric ozone by up to 5 parts per billion, consistent with independent satellite observations. The global total tropospheric ozone burden declined by 6TgO₃ (∼2%) in May and June 2020, largely due to emission reductions in Asia and the Americas that were amplified by regionally high ozone production efficiencies (up to 4 TgO₃/TgN). Our results show that COVID-19 mitigation left a global atmospheric imprint that altered atmospheric oxidative capacity and climate radiative forcing, providing a test of the efficacy of NO_x emissions controls for co-benefiting air quality and climate.

Efforts to stem the spread of COVID‐19 in China hinged on severe restrictions to human movement starting 23 January 2020 in Wuhan and subsequently to other provinces. Here, we quantify the ancillary impacts on air pollution and human health using inverse emissions estimates based on multiple satellite observations. We find that Chinese NOx emissions were reduced by 36% from early January to mid‐February, with more than 80% of reductions occurring after their respective lockdown in most provinces. The reduced precursor emissions increased surface ozone by up to 16 ppb over northern China but decreased PM2.5 by up to 23 μg m⁻³ nationwide. Changes in human exposure are associated with about 2,100 more ozone‐related and at least 60,000 fewer PM2.5‐related morbidity incidences, primarily from asthma cases, thereby augmenting efforts to reduce hospital admissions and alleviate negative impacts from potential delayed treatments.

Global multiconstituent concentration and emission fields obtained from the assimilation of the satellite retrievals of ozone, CO, NO₂, HNO₃, and SO₂ from the Ozone Monitoring Instrument (OMI), Global Ozone Monitoring Experiment 2, Measurements of Pollution in the Troposphere, Microwave Limb Sounder, and Atmospheric Infrared Sounder (AIRS)/OMI are used to understand the processes controlling air pollution during the Korea‐United States Air Quality (KORUS‐AQ) campaign. Estimated emissions in South Korea were 0.42 Tg N for NO_x and 1.1 Tg CO for CO, which were 40% and 83% higher, respectively, than the a priori bottom‐up inventories, and increased mean ozone concentration by up to 7.5 ± 1.6 ppbv. The observed boundary layer ozone exceeded 90 ppbv over Seoul under stagnant phases, whereas it was approximately 60 ppbv during dynamical conditions given equivalent emissions. Chemical reanalysis showed that mean ozone concentration was persistently higher over Seoul (75.10 ± 7.6 ppbv) than the broader KORUS‐AQ domain (70.5 ± 9.2 ppbv) at 700 hPa. Large bias reductions (>75%) in the free tropospheric OH show that multiple‐species assimilation is critical for balanced tropospheric chemistry analysis and emissions. The assimilation performance was dependent on the particular phase. While the evaluation of data assimilation fields shows an improved agreement with aircraft measurements in ozone (to less than 5 ppbv biases), CO, NO₂, SO₂, PAN, and OH profiles, lower tropospheric ozone analysis error was largest at stagnant conditions, whereas the model errors were mostly removed by data assimilation under dynamic weather conditions. Assimilation of new AIRS/OMI ozone profiles allowed for additional error reductions, especially under dynamic weather conditions. Our results show the important balance of dynamics and emissions both on pollution and the chemical assimilation system performance.

We investigate the contributions of emission changes from 10 world regions, as well as the global methane concentration change, on the global tropospheric ozone burden change from 1980 to 2010. The modeled global tropospheric ozone burden has increased by 28.1 Tg, with 26.7% (7.5 Tg) of this change attributed to the global methane increase. Southeast Asia (5.6 Tg) and South Asia (4.0) contribute comparably to the global ozone burden change as East Asia (5.6), even though NO_x emission increases in each region are less than one‐third of those in East Asia, highlighting the greater sensitivity of global ozone to these regions. Emission decreases from North America, Europe, and Former Soviet Union have led to ozone burden decreases of 2.8, 1.0, and 0.3 Tg. The greater sensitivity of the global ozone burden to emission changes in tropical and subtropical regions emphasizes the importance of controlling emissions in these regions for global ozone.

Ambient air pollution from ozone and fine particulate matter is associated with premature mortality. As emissions from one continent influence air quality over others, changes in emissions can also influence human health on other continents. We estimate global air-pollution-related premature mortality from exposure to PM_2.5 and ozone and the avoided deaths due to 20 % anthropogenic emission reductions from six source regions, North America (NAM), Europe (EUR), South Asia (SAS), East Asia (EAS), Russia–Belarus–Ukraine (RBU), and the Middle East (MDE), three global emission sectors, power and industry (PIN), ground transportation (TRN), and residential (RES), and one global domain (GLO), using an ensemble of global chemical transport model simulations coordinated by the second phase of the Task Force on Hemispheric Transport of Air Pollutants (TF HTAP2), and epidemiologically derived concentration response functions. We build on results from previous studies of TF HTAP by using improved atmospheric models driven by new estimates of 2010 anthropogenic emissions (excluding methane), with more source and receptor regions, new consideration of source sector impacts, and new epidemiological mortality functions. We estimate 290 000 (95 % confidence interval (CI): 30 000, 600 000) premature O₃-related deaths and 2.8 million (0.5 million, 4.6 million) PM_2.5-related premature deaths globally for the baseline year 2010. While 20 % emission reductions from one region generally lead to more avoided deaths within the source region than outside, reducing emissions from MDE and RBU can avoid more O₃-related deaths outside of these regions than within, and reducing MDE emissions also avoids more PM_2.5-related deaths outside of MDE than within. Our findings that most avoided O₃-related deaths from emission reductions in NAM and EUR occur outside of those regions contrast with those of previous studies, while estimates of PM_2.5-related deaths from NAM, EUR, SAS, and EAS emission reductions agree well. In addition, EUR, MDE, and RBU have more avoided O₃-related deaths from reducing foreign emissions than from domestic reductions. For six regional emission reductions, the total avoided extra-regional mortality is estimated as 6000 (−3400, 15 500) deaths per year and 25 100 (8200, 35 800) deaths per year through changes in O₃ and PM_2.5, respectively. Interregional transport of air pollutants leads to more deaths through changes in PM_2.5 than in O₃, even though O₃ is transported more on interregional scales, since PM_2.5 has a stronger influence on mortality. For NAM and EUR, our estimates of avoided mortality from regional and extra-regional emission reductions are comparable to those estimated by regional models for these same experiments. In sectoral emission reductions, TRN emissions account for the greatest fraction (26–53 % of global emission reduction) of O₃-related premature deaths in most regions, in agreement with previous studies, except for EAS (58 %) and RBU (38 %) where PIN emissions dominate. In contrast, PIN emission reductions have the greatest fraction (38–78 % of global emission reduction) of PM_2.5-related deaths in most regions, except for SAS (45 %) where RES emission dominates, which differs with previous studies in which RES emissions dominate global health impacts. The spread of air pollutant concentration changes across models contributes most to the overall uncertainty in estimated avoided deaths, highlighting the uncertainty in results based on a single model. Despite uncertainties, the health benefits of reduced intercontinental air pollution transport suggest that international cooperation may be desirable to mitigate pollution transported over long distances.