Spatiotemporal variations of ozone (O₃) and nitrogen oxide (NO_x) mixing ratios from 14 state-of-the-art chemical transport models (CTMs) are intercompared and evaluated with O₃ observations in East Asia, within the framework of the Model Inter-Comparison Study for Asia Phase III (MICS-Asia III). This study was designed to evaluate the capabilities and uncertainties of current CTMs simulations for Asia and to provide multi-model estimates of pollutant distributions. These models were run by 14 independent groups working in China, Japan, South Korea, the United States and other countries/regions. Compared with the previous phase of MICS-Asia (MICS-Asia II), the evaluation with observations was extended from 4 months to 1 full year across China and the western Pacific Rim. In general, model performance levels for O₃ varied widely by region and season. Most models captured the key patterns of monthly and diurnal variation of surface O₃ and its precursors in the North China Plain and western Pacific Rim but failed to do so for the Pearl River Delta. A significant overestimation of surface O₃ was evident from May to September/October and from January to May over the North China Plain, the western Pacific Rim and the Pearl River Delta. Comparisons drawn from observations show that the considerable diversity in O₃ photochemical production partly contributed to this overestimation and to high levels of inter-model variability in O₃ for North China. In terms of O₃ soundings, the ensemble average of models reproduced the vertical structure for the western Pacific, but overestimated O₃ levels to below 800 hPa in the summer. In the industrialized Pearl River Delta, the ensemble average presented an overestimation for the lower troposphere and an underestimation for the middle troposphere. The ensemble average of 13 models for O₃ did not always exhibit superior performance compared with certain individual models in contrast with its superior value for Europe. This finding suggests that the spread of ensemble-model values does not represent all of the uncertainties of O₃ or that most MICS-Asia III models missed key processes. This study improved the performance of modeling O₃ in March at Japanese sites compared with MICS-Asia II. However, it overpredicted surface O₃ concentrations for western Japan in July, which was not found by MICS-Asia II. Major challenges still remain with regard to identifying the sources of bias in surface O₃ over East Asia in CTMs.

Topic 3 of the Model Inter-Comparison Study for Asia (MICS-Asia) Phase III examines how online coupled air quality models perform in simulating high aerosol pollution in the North China Plain region during wintertime haze events and evaluates the importance of aerosol radiative and microphysical feedbacks. A comprehensive overview of the MICS-Asia III Topic 3 study design, including descriptions of participating models and model inputs, the experimental designs, and results of model evaluation, are presented. Six modeling groups from China, Korea and the United States submitted results from seven applications of online coupled chemistry–meteorology models. Results are compared to meteorology and air quality measurements, including data from the Campaign on Atmospheric Aerosol Research Network of China (CARE-China) and the Acid Deposition Monitoring Network in East Asia (EANET). The correlation coefficients between the multi-model ensemble mean and the CARE-China observed near-surface air pollutants range from 0.51 to 0.94 (0.51 for ozone and 0.94 for PM_2.5) for January 2010. However, large discrepancies exist between simulated aerosol chemical compositions from different models. The coefficient of variation (SD divided by the mean) can reach above 1.3 for sulfate in Beijing and above 1.6 for nitrate and organic aerosols in coastal regions, indicating that these compositions are less consistent from different models. During clean periods, simulated aerosol optical depths (AODs) from different models are similar, but peak values differ during severe haze events, which can be explained by the differences in simulated inorganic aerosol concentrations and the hygroscopic growth efficiency (affected by varied relative humidity). These differences in composition and AOD suggest that future models can be improved by including new heterogeneous or aqueous pathways for sulfate and nitrate formation under hazy conditions, a secondary organic aerosol (SOA) formation chemical mechanism with new volatile organic compound (VOCs) precursors, yield data and approaches, and a more detailed evaluation of the dependence of aerosol optical properties on size distribution and mixing state. It was also found that using the ensemble mean of the models produced the best prediction skill. While this has been shown for other conditions (for example, the prediction of high-ozone events in the US (McKeen et al., 2005)), this is to our knowledge the first time it has been shown for heavy haze events.

Despite the significant progress in improving chemical transport models (CTMs), applications of these modeling endeavors are still subject to large and complex model uncertainty. The Model Inter-Comparison Study for Asia III (MICS-Asia III) has provided the opportunity to assess the capability and uncertainty of current CTMs in East Asian applications. In this study, we have evaluated the multi-model simulations of nitrogen dioxide (NO₂), carbon monoxide (CO) and ammonia (NH₃) over China under the framework of MICS-Asia III. A total of 13 modeling results, provided by several independent groups from different countries and regions, were used in this study. Most of these models used the same modeling domain with a horizontal resolution of 45 km and were driven by common emission inventories and meteorological inputs. New observations over the North China Plain (NCP) and Pearl River Delta (PRD) regions were also available in MICS-Asia III, allowing the model evaluations over highly industrialized regions. The evaluation results show that most models captured the monthly and spatial patterns of NO₂ concentrations in the NCP region well, though NO₂ levels were slightly underestimated. Relatively poor performance in NO₂ simulations was found in the PRD region, with larger root-mean-square error and lower spatial correlation coefficients, which may be related to the coarse resolution or inappropriate spatial allocations of the emission inventories in the PRD region. All models significantly underpredicted CO concentrations in both the NCP and PRD regions, with annual mean concentrations that were 65.4 % and 61.4 % underestimated by the ensemble mean. Such large underestimations suggest that CO emissions might be underestimated in the current emission inventory. In contrast to the good skills for simulating the monthly variations in NO₂ and CO concentrations, all models failed to reproduce the observed monthly variations in NH₃ concentrations in the NCP region. Most models mismatched the observed peak in July and showed negative correlation coefficients with the observations, which may be closely related to the uncertainty in the monthly variations in NH₃ emissions and the NH₃ gas–aerosol partitioning. Finally, model intercomparisons have been conducted to quantify the impacts of model uncertainty on the simulations of these gases, which are shown to increase with the reactivity of species. Models contained more uncertainty in the NH₃ simulations. This suggests that for some highly active and/or short-lived primary pollutants, like NH₃, model uncertainty can also take a great part in the forecast uncertainty in addition to the emission uncertainty. Based on these results, some recommendations are made for future studies.

Space-borne ozone (O₃) measurements have indicated consistent positive trends across the entire Asia–Pacific region despite the considerable reduction of NO_x since 2000s. The rate of increase in O₃ derived from lower free tropospheric column measurements was observed to be 0.21 ± 0.05 DU/decade during 2005–2018. Our space-borne-based diagnosis of the nonlinear photochemical formation regimes, NO_x-limited and NO_x-saturated, show that O₃ chemistry is undergoing a transitional process to the NO_x-limited regime throughout most of the Asian region. Nevertheless, NO_x-saturated conditions persist at present in and over eight major megacities. These NO_x-saturated conditions in megacities contribute to the increased O₃ due to NO_x reduction, which could also affect the enhanced O₃ concentrations throughout the Asia–Pacific region via long-range transport. This indicates that VOC limits along with NO_x reductions are needed in megacities in the short term to reduce O₃ levels. Moreover, NO_x saturation in major megacities will continue until 2025, according to the forecast emission scenarios from the Intergovernmental Panel on Climate Change (IPCC). These scenarios gradually shift nearly all cities to the NO_x-limited regime by 2050 with the exception of few cities under IPCC RCP8.5. Thus, continued reductions in NO_x will be a key factor in reducing O₃ in the long term.

Urban photochemical ozone (O₃) formation regimes (NO_x- and VOC-limited regimes) at nine megacities in East Asia were diagnosed based on near-surface O₃ columns from 900 to 700 hPa, nitrogen dioxide (NO₂), and formaldehyde (HCHO), which were inferred from measurements by ozone-monitoring instruments (OMI) for 2014–2018. The nine megacities included Beijing, Tianjin, Hebei, Shandong, Shanghai, Seoul, Busan, Tokyo, and Osaka. The space-borne HCHO–to–NO₂ ratio (FNR) inferred from the OMI was applied to nine megacities and verified by a series of sensitivity tests of Weather Research and Forecasting model with Chemistry (WRF-Chem) simulations by halving the NO_x and VOC emissions. The results showed that the satellite-based FNRs ranged from 1.20 to 2.62 and the regimes over the nine megacities were identified as almost NO_x-saturated conditions, while the domain-averaged FNR in East Asia was >2. The results of WRF–Chem sensitivity modeling show that O₃ increased when the NO_x emissions reduced, whereas VOC emission reduction showed a significant decrease in O₃, confirming the characteristics of VOC-limited conditions in all of the nine megacities. When both NOx and VOC emissions were reduced, O₃ decreased in most cities, but increased in the three lowest-FNRs megacities, such as Shanghai, Seoul, and Tokyo, where weakened O₃ titration caused by NOx reduction had a larger enough effect to offset O₃ suppression induced by the decrease in VOCs. Our model results, therefore, indicated that the immediate VOC emission reduction is a key controlling factor to decrease megacity O₃ in East Asia, and also suggested that both VOC and NO_x reductions may not be of broad utility in O₃ abatement in megacities and should be considered judiciously in highly NO_x-saturated cities in East Asia.

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 ${\mathrm{SO}}_{\mathrm{4}}^{\mathrm{2}-}$ 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).