An Inversion of NOx and NMVOC Emissions using Satellite Observations during the KORUS-AQ Campaign and Implications for Surface Ozone over East Asia

The absence of up-to-date emissions has been a major impediment to accurately simulate aspects of atmospheric chemistry, and to precisely quantify the impact of changes of emissions on air pollution. Hence, a non-linear joint analytical inversion (Gauss-Newton method) of both volatile organic compounds (VOC) and nitrogen oxides (NOx) emissions is made by exploiting the Smithsonian Astrophysical Observatory (SAO) Ozone Mapping and Profile Suite 25 Nadir Mapper (OMPS-NM) formaldehyde (HCHO) and the National Aeronautics and Space Administration (NASA) Ozone Monitoring Instrument (OMI) tropospheric nitrogen dioxide (NO2) retrievals during the Korea-United States Air Quality (KORUS-AQ) campaign over East Asia in May-June 2016. Effects of the chemical feedback of NOx and VOCs on both NO2 and HCHO are implicitly included through iteratively optimizing the inversion. Emissions estimates 30 are greatly improved (averaging kernels>0.8) over medium-to high-emitting areas such as cities and dense vegetation. The amount of total NOx emissions is mainly dictated by values reported in the MIX-Asia 2010 inventory. After the inversion we conclude a decline in the emissions (before, after, change) for China (87.94±44.09 Gg/day, 68.00±15. 2 Gg/day,-41%), Taiwan (1.26±0.57 Gg/day, 0.97±0.33 Gg/day,-23%), and Malaysia (2.89±2.77 Gg/day, 2.25±1.34 Gg/day,-22%), all of which have effectively implemented various stringent regulations. In contrast, South Korea (2.71±1.34 Gg/day, 2.95±0.58 Gg/day, +9%) and Japan (3.53±1.71 Gg/day, 3.96±1.04 Gg/day, +12%) experience an increase in NOx emissions potentially 40 due to risen number of diesel vehicles and new thermal power plants. We revisit the well-documented positive bias of the model in terms of biogenic VOC emissions in the tropics. The inversion, however, suggests a larger growth of VOC (mainly anthropogenic) over NCP (25%) than previously reported (6%) relative to 2010. The spatial variation in both magnitude and sign of NOx and VOC emissions results in non-linear responses of ozone production/loss. Due to 45 simultaneous decrease/increase of NOx/VOC over NCP and YRD, we observe an ~53% reduction in the ratio of the chemical loss of NOx (LNOx) to the chemical loss of ROx (RO2+HO2) transitioning toward NOx-sensitive regimes, which in turn, reduces/increases the afternoon chemical loss/production of ozone through NO2+OH (-0.42 ppbv hr-1)/HO2 (and RO2)+NO (+0.31 ppbv hr-1). Conversely, a combined decrease in NOx and VOC emissions in Taiwan, Malaysia, and 50 the southern China suppresses the formation of ozone. Ultimately, model simulations indicate enhancements of maximum daily 8-hour average (MDA8) surface ozone over China (0.62 ppbv), NCP (4.56 ppbv), and YRD (5.25 ppbv) due to the non-linear ozone chemistry, suggesting that emissions standards should be extended to regulate VOCs to be able to curb ozone production rates. Taiwan, Malaysia, and PRD stand out as the regions undergoing lower MDA8 ozone levels 55 resulting from the NOx reductions occurring predominantly in NOx-sensitive regimes