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The concentration of carbonaceous aerosols, black carbon (BC) and organic aerosol (OA), in the atmosphere is related to co-emitted or co-produced trace gases. In this study, we investigate the most relevant proportional relationships between both BC and OA with the following trace gases: carbon monoxide (CO), formaldehyde (HCHO), nitrogen dioxide (NO2), ozone (O3), and sulfur dioxide (SO2). One motivation for selecting these trace gases is that they can be observed using remote sensing measurements from satellite instrumentation, and could therefore be used to predict spatial changes in the amounts of BC and OA. Airborne measurements are optimal for the analysis of both the composition of aerosols and trace gases in different environments ranging from unpolluted oceanic air masses to those in heavily polluted city plumes. The two aircraft campaigns of the EMeRGe (Effect of Megacities on the Transport and Transformation of Pollutants on the Regional to Global Scales) project have created a unique database, with flight plans dedicated to studying city plumes in two regions, Europe (2017) and East Asia (2018), along with identical instrumental payload. Using linear regression analysis, three relevant relationships between carbonaceous aerosol and trace gases are identified: - The BC/OA ratio observed in the Asian campaign is three times higher (≈ 0.3) than in the European campaign (≈ 0.1), whereas the Pearson correlation coefficient (R) between BC and OA is much higher in Europe (R ≈ 0.8) than in Asia (R ≈ 0.6). - The CO/BC ratio is also observed higher in the Asian campaign (≈ 240) than in the European campaign (≈ 170), whereas the R-value between CO and BC is similar for both campaigns (R ≈ 0.7). - The HCHO/OA ratio is similar in both campaigns (≈0.32), but the observed R-values between HCHO and OA is higher in Europe than in the Asia (R ≈ 0.7 compared to ≈ 0.3). By focusing on heavily polluted air masses sampled downwind in the city plumes, the ratios between the observed carbonaceous aerosols and the five trace gases change, and the R-values increase with O3 for both BC and OA (R ≈ 0.5). To assess the performance of atmospheric models with respect to the most relevant observed relationships, an air quality model ensemble is used to represent the current state of atmospheric modeling, consisting of two global and two regional simulations. The evaluation shows that these proportional relationships are not satisfactorily reproduced by the model ensemble. The relationships between BC and OA or between CO and BC are modeled with stronger correlations than the observed ones, and their higher ratios observed in Asia compared to Europe are not reproduced. Furthermore, the modeled HCHO/OA ratio is underestimated in the Asian campaign and overestimated in the European campaign. This analysis of the proportional relationships between carbonaceous aerosols and trace gases implies that the observed relationships can be used to constrain models and improve anthropogenic emission inventories. In addition, it implies that information about the lower tropospheric concentration of carbonaceous aerosols can potentially be inferred from satellite retrievals of trace gases, particularly in the plumes from megacities. [ABSTRACT FROM AUTHOR]

Nitrous acid (HONO) is an important atmospheric gas given its contribution to the cycles of NO x and HO x , but its role in global atmospheric photochemistry is not fully understood. This study implemented three pathways of HONO formation in the chemistry–climate model CHASER (MIROC-ESM) to explore three physical phenomena: gas-phase kinetic reactions (GRs), direct emission (EM), and heterogeneous reactions on cloud and aerosol particles (HRs). We evaluated the simulations by the atmospheric aircraft-based measurements from EMeRGe-Asia-2018 (Effect of Megacities on the Transport and Transformation of Pollutants on the Regional to Global Scales), ATom-1 (atmospheric tomography), observations from the ship R/V Mirai, EANET (Acid Deposition Monitoring Network in eastern Asia)/EMEP (European Monitoring and Evaluation Programme) ground-based stationary observations, and the OMI (Ozone Monitoring Instrument). We showed that the inclusion of the HONO chemistry in the modelling process reduced the model bias against the measurements for PM 2.5 , NO 3- /HNO 3 , NO 2 , OH, HO 2 , O 3 , and CO, especially in the lower troposphere and the North Pacific (NP) region. We found that the retrieved global abundance of tropospheric HONO was 1.4 TgN. Of the three source pathways, HRs and EM contributed 63 % and 26 % to the net HONO production, respectively. We also observed that reactions on the aerosol surfaces contributed larger amounts of HONO (51 %) than those on the cloud surfaces (12 %). The model exhibited significant negative biases for daytime HONO in the Asian off-the-coast region, compared with the airborne measurements by EMeRGe-Asia-2018, indicating the existence of unknown daytime HONO sources. Strengthening of aerosol uptake of NO 2 near the surface and in the middle troposphere, cloud uptake, and direct HONO emission were all potential yet-unknown HONO sources. The most promising daytime source for HONO found in this study was the combination of enhanced aerosol uptake of NO 2 and surface-catalysed HNO 3 photolysis (maxST + JANO3-B case), which could also remedy the model bias for NO 2 and O 3 during EMeRGe. We also found that the simulated HONO abundance and its impact on NO x –O 3 chemistry were sensitive to the yield of the heterogeneous conversion of NO 2 to HONO (vs. HNO 3). Inclusion of HONO reduced global tropospheric NO x (NO + NO 2) levels by 20.4 %, thereby weakening the tropospheric oxidizing capacity (OH, O 3) occurring for NO x -deficit environments (remote regions and upper altitudes), which in turn increased CH 4 lifetime (13 %) and tropospheric CO abundance (8 %). The calculated reduction effect on the global ozone level reduced the model overestimates for tropospheric column ozone against OMI spaceborne observations for a large portion of the North Hemisphere. HRs on the surfaces of cloud particles, which have been neglected in previous modelling studies, were the main drivers of these impacts. This effect was particularly salient for the substantial reductions of levels of OH (40 %–67 %) and O 3 (30 %–45 %) in the NP region during summer, given the significant reduction of the NO x level (50 %–95 %). In contrast, HRs on aerosol surfaces in China (Beijing) enhanced OH and O 3page928 winter mean levels by 600 %–1700 % and 10 %–33 %, respectively, with regards to their minima in winter. Furthermore, sensitivity simulations revealed that the heterogeneous formation of HONO from NO 2 and heterogenous photolysis of HNO 3 coincided in the real atmosphere. Nevertheless, the global effects calculated in the combined case (enhancing aerosol uptakes of NO 2 and implementing heterogeneous photolysis of HNO 3), which most captured the measured daytime HONO level, still reduced the global tropospheric oxidizing capacity. Overall, our findings suggest that a global model that does not consider HONO heterogeneous mechanisms (especially photochemical heterogeneous formations) may erroneously predict the effect of HONO in remote areas and polluted regions. [ABSTRACT FROM AUTHOR]

Combined NO2 and CO2 observations have the potential to constrain the identification of the locations and strength of urban CO2 emissions, in particular, point sources such as power plants. We report the first results of airborne spectroscopic NO2 and CO2 observations over an urban area in Japan in February 2018. Inversed emission rates of two stacks of the coal‐fired power plant for CO2 showed relatively good agreement with those estimated by a bottom‐up inventory—the Regional Emission inventory in ASia (REAS) v3.1—within −7% to 40% because the plume shapes were well identified due to constraint by NO2 measurements. The estimated NOx emission rates showed discrepancies more than 80% with those estimated by the REAS v3.1, mainly due to the uncertainties in activity data and emission factors, or in the greatly varying NO/NO2 ratios in fresh plumes, which warrant further investigations when estimating NOx emissions from satellite NO2 observations on km‐scales. Plain Language Summary: Burning of fossil fuels at high temperatures constitutes a major anthropogenic source of nitrogen oxides (NOx) and carbon dioxide (CO2). While CO2 stays in the atmosphere for hundreds of years, thereby being a well‐mixed gas, NO2 has a much shorter lifetime of only a few hours. This substantial difference in lifetime between NO2 and CO2 means that concurrent NO2 and CO2 observations obtained by the same platform can be used to identify the locations and strength of CO2 emissions from point sources such as power plants. In February 2018, for the first time, we obtained concurrent airborne spectroscopic NO2 and CO2 observations over an urban area, to demonstrate the traceability of NO2 to CO2. The plumes of co‐emitted NO2 and CO2 were derived from measured spectra. The plumes of NO2 and CO2 co‐emitted from the stacks of power plants were well identified owing to constraint by NO2. Uncertainties of inversed emission rates were statistically derived. For CO2, the results were within 40% in agreement with a bottom‐up emission inventory known as REAS v3.1. For NOx, however, a disagreement of 80% was identified, likely due to the uncertainties of the inventory data or in the NOx partitioning in fresh plumes. Key Points: Concurrent observations of NO2 and CO2 in fresh plumes from a large single point source using airborne spectrometers were reportedColumnar enhancements of NO2 and CO2 due to power plant emissions were up to 3.8 × 1016 molec.cm−2 and 75 ppm, respectivelyPlume shapes of CO2 emitted from power plants were well identified and constrained by NO2 plume shapes [ABSTRACT FROM AUTHOR]