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This study describes the application of a regional Earth system model with updated parameterizations for selected land–atmosphere exchange processes and multiplatform, multidisciplinary observations. We estimate reactive nitrogen (Nr = NO y+ NHx) emissions from various sources, surface and column nitrogen dioxide (NO2), and total and speciated Nr dry and wet deposition during 2018–2023 over the northeastern and mid-Atlantic US where nitrogen-oxide-limited or transitional chemical regimes dominate. The estimated Nr concentrations and deposition fluxes are related to ozone (O3) in terms of spatiotemporal variability and its key drivers as well as possible ecosystem impacts. Modeled surface O3 persistently agrees well with observations, with root mean square errors staying within 4–7 ppbv for individual years in May–June–July. Model-based surface O3–NO2 column correlation, which shows a dependency on column formaldehyde / NO2, is higher in 2020 (r=0.62) than in other years (r=0.47 –0.56). Ozone vegetative uptake overall dropped by ∼10% from 2018 to 2023, displaying clearer downward temporal changes than total Nr deposition as declining NOy emission and deposition competed with increasing NHx fluxes. It is highlighted that temporal variabilities of Nr and O3 concentrations and fluxes on subregional to local scales respond to hydrological variability that can be influenced by precipitation and controllable human activities like irrigation. Deposition and biogenic emissions that are highly sensitive to interconnected environmental and plant physiological conditions, plus extra-regional sources (e.g., O3-rich stratospheric air and dense wildfire plumes from upwind regions), have been playing increasingly important roles in controlling pollutant budgets as local emissions decline owing to effective emission regulations and COVID lockdowns. [ABSTRACT FROM AUTHOR]

Formaldehyde (HCHO) in the atmosphere is an intermediate product from the oxidation of methane and non-methane volatile organic compounds. In remote marine regions, HCHO variability is closely related to atmospheric oxidation capacity, and modeled HCHO in these regions is usually added as a global satellite HCHO background. Thus, it is important to understand and validate the levels of satellite HCHO over the remote oceans. Here we intercompare three satellite retrievals of total HCHO columns from the Ozone Monitoring Instrument Smithsonian Astrophysical Observatory (OMI SAO (v004)) algorithm, Ozone Mapping and Profiler Suite on Suomi National Polar-orbiting Partnership Smithsonian Astrophysical Observatory (OMPS-NPP SAO) algorithm, and Ozone Monitoring Instrument Belgian Institute for Space Aeronomy (OMI BIRA) algorithm and validate them against in situ observations from the NASA Atmospheric Tomography Mission (ATom) mission. All retrievals are correlated with ATom-integrated columns over remote oceans, with OMI SAO (v004) showing the best agreement. This is also reflected in the mean bias (MB) for OMI SAO (- 0.73 ± 0.87) × 1015 molec. cm−2, OMPS SAO (- 0.76 ± 0.88) × 1015 molec. cm−2, and OMI BIRA (- 1.40 ± 1.11) × 1015 molec. cm−2. We recommend the OMI-SAO (v004) retrieval for remote-ocean atmosphere studies. Three satellite HCHO retrievals and in situ ATom columns all generally captured the spatial and seasonal distributions of HCHO in the remote-ocean atmosphere. Retrieval bias varies by latitude and season, but a persistent low bias is found in all products at high latitudes, and the general low bias is most severe for the OMI BIRA product. Examination of retrieval components reveals that slant column corrections have a larger impact on the retrievals over remote marine regions, while AMFs play a smaller role. This study informs us that the potential latitude-dependent biases in the retrievals require further investigation for improvement and should be considered when using marine HCHO satellite data, and vertical profiles from in situ instruments are crucial for validating satellite retrievals. [ABSTRACT FROM AUTHOR]

Temperature is the principal driver of global atmospheric formaldehyde (HCHO) and its primary oxidation precursor biogenic volatile organic compounds (BVOCs). We revisit such a temperature (T‐) dependency globally, leveraging TROPOMI HCHO column data. We find substantial variations in the T‐dependency of biogenic HCHO across plant functional types (PFTs), with the highest over Broadleaf Evergreen Tropical Trees (doubling every 6.0 K ± 4.1 K) and lowest over Arctic C3 Grass (doubling every 30.8 K ± 9.6 K). The GEOS‐Chem model interprets HCHO columns' T‐dependency at the PFT level (r = 0.87), with a 16% discrepancy on average. The discrepancy can be explained by BVOC emissions T‐dependency for Broadleaf Evergreen Tropical Trees and Warm C4 Grass and can be attributed to the insensitivity of HCHO columns to BVOC emissions for other PFTs. Our findings underscore a potentially magnified variation of BVOC emissions by GEOS‐Chem and MEGAN therein, particularly in regions experiencing greater temperature variations. Plain Language Summary: We use remote sensing data from an up‐to‐date monitor to examine the temperature (T‐) dependency of biogenic formaldehyde (HCHO), a proxy of a series of volatile organic gases released by plants, in a global manner. We find that the effect of temperature on HCHO varies significantly between different types of plants, with tropical evergreen trees showing the most sensitivity to temperature and Arctic grasses showing the least. The GEOS‐Chem, a state‐of‐the‐art chemical transport model, interprets such temperature sensitivity among plants with nonnegligible discrepancies. The sensitivity of volatile organic gases released by plants to temperature explains the sensitivity of HCHO to temperature for some plants, such as tropical evergreen trees and warm‐season grasses. Key Points: Temperature (T‐) dependency of biogenic HCHO columns varies substantially across plant functional types (PFTs)The GEOS‐Chem model with the MEGAN module implemented primarily interprets the T‐dependency of HCHO columns at the PFT levelThe T‐dependency of biogenic volatile organic compound (BVOC) emissions mainly accounts for that of HCHO columns in Broadleaf Evergreen Tropical Trees and Warm C4 Grass regions [ABSTRACT FROM AUTHOR]

Tropospheric ozone results from in situ chemical formation and stratosphere–troposphere exchange (STE), with the latter being more important in the middle and upper troposphere than in the lower troposphere. Ozone photochemical formation is nonlinear and results from the oxidation of methane and non-methane hydrocarbons (NMHCs) in the presence of nitrogen oxide (NO x= NO + NO2). Previous studies showed that O3 short- and long-term trends are nonlinearly controlled by near-surface anthropogenic emissions of carbon monoxide (CO), volatile organic compounds (VOCs), and nitrogen oxides, which may also be impacted by the long-range transport (LRT) of O3 and its precursors. In addition, several studies have demonstrated the important role of STE in enhancing ozone levels, especially in the midlatitudes. In this article, we investigate tropospheric ozone spatial variability and trends from 2005 to 2019 and relate those to ozone precursors on global and regional scales. We also investigate the spatiotemporal characteristics of the ozone formation regime in relation to ozone chemical sources and sinks. Our analysis is based on remote sensing products of the tropospheric column of ozone (TrC-O3) and its precursors, nitrogen dioxide (TrC-NO2), formaldehyde (TrC-HCHO), and total column CO (TC-CO), as well as ozonesonde data and model simulations. Our results indicate a complex relationship between tropospheric ozone column levels, surface ozone levels, and ozone precursors. While the increasing trends of near-surface ozone concentrations can largely be explained by variations in VOC and NOx concentration under different regimes, TrC-O3 may also be affected by other variables such as tropopause height and STE as well as LRT. Decreasing or increasing trends in TrC-NO2 have varying effects on TrC-O3, which is related to the different local chemistry in each region. We also shed light on the contribution of NOx lightning and soil NO and nitrous acid (HONO) emissions to trends of tropospheric ozone on regional and global scales. [ABSTRACT FROM AUTHOR]

The Geostationary Environment Monitoring Spectrometer (GEMS) on board the GEO-KOMPSAT-2B satellite is the first geostationary satellite launched to monitor the environment. GEMS conducts hourly measurements during the day over eastern and southeastern Asia. This work presents glyoxal (CHOCHO) vertical column densities (VCDs) retrieved from GEMS, with optimal settings for glyoxal retrieval based on sensitivity tests involving reference spectrum sampling and fitting window selection. We evaluated GEMS glyoxal VCDs by comparing them to the TROPOspheric Monitoring Instrument (TROPOMI) and multi-axis differential optical absorption spectroscopy (MAX-DOAS) ground-based observations. On average, GEMS and TROPOMI VCDs show a spatial correlation coefficient of 0.63, increasing to 0.87 for northeastern Asia. While GEMS and TROPOMI demonstrate similar monthly variations in the Indochinese Peninsula regions (R > 0.67), variations differ in other areas. Specifically, GEMS VCDs are higher in the winter and either lower or comparable to TROPOMI and MAX-DOAS VCDs in the summer across northeastern Asia. We attributed the discrepancies in the monthly variation to a polluted reference spectrum and high NO2 concentrations. When we correct GEMS glyoxal VCDs as a function of NO2 SCDs, the monthly correlation coefficients substantially increase from 0.16–0.40 to 0.45–0.72 in high NO2 regions. When averaged hourly, GEMS and MAX-DOAS VCDs exhibit similar diurnal variations, especially at stations in Japan (Chiba, Kasuga, and Fukue). [ABSTRACT FROM AUTHOR]

The Geostationary Environment Monitoring Spectrometer (GEMS) on board GEO-KOMPSAT-2B was launched in February 2020 and has been monitoring atmospheric chemical compositions over Asia. We present the first evaluation of the operational GEMS formaldehyde (HCHO) vertical column densities (VCDs) during and after the in-orbit test (IOT) period (August–October 2020) by comparing them with the products from the TROPOspheric Monitoring Instrument (TROPOMI) and Fourier-transform infrared (FTIR) and multi-axis differential optical absorption spectroscopy (MAX-DOAS) instruments. During the IOT, the GEMS HCHO VCDs reproduced the observed spatial pattern of TROPOMI VCDs over the entire domain (r= 0.62) with high biases (10 %–16 %). We found that the agreement between GEMS and TROPOMI was substantially higher in Northeast Asia (r= 0.90), encompassing the Korean Peninsula and east China. GEMS HCHO VCDs captured the seasonal variation in HCHO, primarily driven by biogenic emissions and photochemical activities, but showed larger variations than those of TROPOMI over coastal regions (Kuala Lumpur, Singapore, Shanghai, and Busan). In addition, GEMS HCHO VCDs showed consistent hourly variations with MAX-DOAS (r= 0.77) and FTIR (r= 0.86) but were 30–40 % lower than ground-based observations. Different vertical sensitivities of GEMS and ground-based instruments caused these biases. Utilizing the averaging kernel smoothing method reduces the low biases by approximately 10 % to 15 % (normalized mean bias (NMB): - 47.4 % to - 31.5 % and - 38.6 % to - 26.7 % for MAX-DOAS and FTIR, respectively). The remaining discrepancies are due to multiple factors, including spatial collocation and different instrumental sensitivities, requiring further investigation using inter-comparable datasets. [ABSTRACT FROM AUTHOR]

This study applies a regional Earth system model (NASA-Unified Weather Research and Forecasting with online chemistry) with updated parameterizations for selected land-air exchange processes and multi-platform observations, to first estimate reactive nitrogen (Nr = oxidized NOy + reduced NHx) emissions from anthropogenic and natural sources, nitrogen dioxide (NO2) column densities and surface concentrations, total and speciated Nr dry or/and wet deposition fluxes during 2018-2023 over the northeastern and Mid-Atlantic US most of which belong to nitrogen oxides-limited or transitional chemical regimes. The estimated multi-year Nr concentrations and deposition fluxes are then compared with and related to ozone (O3), in terms of their spatiotemporal variability and key drivers as well as possible ecosystem impacts. Finally, through three sets of case studies, we identify and discuss about 1) the capability of land data assimilation (DA) to reduce the uncertainty in modeled land surface states at daily-to-interannual timescales, that can propagate into atmospheric chemistry fields; 2) the impacts of irrigation on land surface and atmospheric fields as well as pollutants' ecosystem uptake and impacts; and 3) the impacts of transboundary air pollution during selected extreme events on pollutants' budgets and ecosystem impacts. With the updated model parameterizations and anthropogenic emission inputs, the eastern US surface O3 modeled by this tool persistently agrees better with observations (i.e., with root-mean-square errors staying within 4-7 ppbv for the individual years' May-June-July) than those in literature where model errors often exceed 20 ppbv. Based on model calculations, surface O3 correlates more strongly with early afternoon NO2 columns than formaldehyde columns (r=0.54 and 0.40, respectively). The O3 vegetative uptake overall dropped by ~10% from 2018 to 2023, displaying clearer downward temporal changes than the total Nr deposition due to the declining NOy emission and deposition fluxes competing with the increasing NHx fluxes. It is highlighted that, temporal variability of Nr and O3 concentrations and fluxes on subregional-to-local scales respond to hydrological variability that can be influenced by precipitation and controllable human activities such as irrigation. Deposition processes and biogenic emissions that are highly sensitive to interconnected environmental and plants' physiological conditions, as well as extra-regional sources (e.g., O3-rich stratospheric air and dense wildfire plumes from upwind regions), have been playing increasingly important roles in controlling pollutants' budgets in this area as local emissions go down owing to effective emission regulations and COVID lockdowns. To better inform the design of mitigation and adaptation strategies, it is recommended to continue evaluating and improving the model parameterizations and inputs relevant to these processes in seamlessly coupled multiscale Earth system models using laboratory and field experiments in combination with satellite DA which would in turn benefit remote sensing communities. [ABSTRACT FROM AUTHOR]

Spaceborne formaldehyde (HCHO) measurements constitute an excellent proxy for the sources of non-methane volatile organic compounds (NMVOCs). Past studies suggested substantial overestimations of NMVOC emissions in state-of-the-art inventories over major source regions. Here, the QA4ECV (Quality Assurance for Essential Climate Variables) retrieval of HCHO columns from OMI (Ozone Monitoring Instrument) is evaluated against (1) FTIR (Fourier-transform infrared) column observations at 26 stations worldwide and (2) aircraft in situ HCHO concentration measurements from campaigns conducted over the USA during 2012–2013. Both validation exercises show that OMI underestimates high columns and overestimates low columns. The linear regression of OMI and aircraft-based columns gives ΩOMI=0.651Ωairc+2.95×1015 molec.cm-2 , with ΩOMI and Ωairc the OMI and aircraft-derived vertical columns, whereas the regression of OMI and FTIR data gives ΩOMI=0.659ΩFTIR+2.02×1015 molec.cm-2. Inverse modelling of NMVOC emissions with a global model based on OMI columns corrected for biases based on those relationships leads to much-improved agreement against FTIR data and HCHO concentrations from 11 aircraft campaigns. The optimized global isoprene emissions (∼445Tgyr-1) are 25% higher than those obtained without bias correction. The optimized isoprene emissions bear both striking similarities and differences with recently published emissions based on spaceborne isoprene columns from the CrIS (Cross-track Infrared Sounder) sensor. Although the interannual variability of OMI HCHO columns is well understood over regions where biogenic emissions are dominant, and the HCHO trends over China and India clearly reflect anthropogenic emission changes, the observed HCHO decline over the southeastern USA remains imperfectly elucidated. [ABSTRACT FROM AUTHOR]

Volatile organic compounds (VOCs) are key precursors of particulate matter and tropospheric ozone. Although the terrestrial biosphere is by far the largest source of VOCs into the atmosphere, the emissions of biogenic VOCs remain poorly constrained at the regional scale. In this work, we derive top-down biogenic emissions over Europe using weekly averaged TROPOMI formaldehyde (HCHO) data from 2018 to 2021. The systematic bias of the TROPOMI HCHO columns is characterized and corrected for based on comparisons with FTIR data at seven European stations. The top-down fluxes of biogenic, pyrogenic, and anthropogenic VOC sources are optimized using an inversion framework based on the MAGRITTEv1.1 chemistry transport model and its adjoint. The inversion leads to strongly increased isoprene emissions with respect to the MEGAN–MOHYCAN inventory over the model domain (from 8.1 to 18.5 Tgyr-1), which is driven by the high observed TROPOMI HCHO columns in southern Europe. The impact of the inversion on biomass burning VOCs (+ 13 %) and anthropogenic VOCs (- 17 %) is moderate. An evaluation of the optimized HCHO distribution against ground-based remote sensing (FTIR and MAX-DOAS) and in situ data provides generally improved agreement at stations below about 50 ∘ N but indicates overestimated emissions in northern Scandinavia. Sensitivity inversions show that the top-down emissions are robust with respect to changes in the inversion settings and in the model chemical mechanism, leading to differences of up to 10 % in the total emissions. However, the top-down emissions are very sensitive to the bias correction of the observed columns, as the biogenic emissions are 3 times lower when the correction is not applied. Furthermore, the use of different a priori biogenic emissions has a significant impact on the inversion results due to large differences among bottom-up inventories. The sensitivity run using CAMS-GLOB-BIOv3.1 as a priori emissions in the inversion results in 30 % lower emissions with respect to the optimization using MEGAN–MOHYCAN. In regions with large temperature and cloud cover variations, there is strong week-to-week variability in the observed HCHO columns. The top-down emissions, which are optimized at weekly increments, have a much improved capability of representing these large fluctuations than an inversion using monthly increments. [ABSTRACT FROM AUTHOR]

Spaceborne formaldehyde (HCHO) measurements constitute an excellent proxy for the sources of non-methane volatile organic compounds (NMVOCs). Past studies suggested substantial overestimations of NMVOC emission in state-of-the-art inventories over major source regions. Here, the QA4ECV (Quality Assurance for Essential Climate Variables) retrieval of HCHO columns from OMI (Ozone Monitoring Instrument) are evaluated against (1) FTIR (Fourier-transform infrared) column observations at 26 stations worldwide, and (2) aircraft in situ HCHO concentration measurements from campaigns conducted over the U.S. in 2012-2013. Both validation exercises show that OMI underestimates high columns and overestimates low columns. The linear regression of OMI and aircraft-based columns gives OMI = 0.651 airc +2.95 · 1015 molec.cm-2, with OMI and airc the OMI and aircraft-derived vertical columns, whereas the regression of OMI and FTIR data gives OMI = 0.659 FTIR +2.02 · 1015 molec.cm-2. Inverse modelling of NMVOC emissions with a global model based on OMI columns corrected for biases based on those relationships leads to much-improved agreement against FTIR data and HCHO concentrations from 11 aircraft campaigns. The optimized global isoprene emissions (- 445Tg yr-1) are 25% higher than those obtained without bias correction. The optimized isoprene emissions bear both striking similarities and differences with recently published emissions based on spaceborne isoprene columns from the CrIS (Cross-track Infrared Sounder) sensor. Although the interannual variability of OMI HCHO columns is well understood over regions where biogenic emissions are dominant, and the HCHO trends over China and India clearly reflect anthropogenic emission changes, the observed HCHO decline over the Southeastern U.S. remains imperfectly elucidated. [ABSTRACT FROM AUTHOR]

Volatile organic compounds (VOCs) are key precursors of particulate matter and tropospheric ozone. Although the terrestrial biosphere is by far the largest source of VOCs into the atmosphere, the emissions of biogenic VOCs remain poorly constrained at regional scale. In this work, we derive top-down biogenic emissions over Europe using weekly-averaged TROPOMI formaldehyde (HCHO) data from 2018 to 2021. The systematic bias of the TROPOMI HCHO columns is characterized and corrected for based on comparisons with FTIR data at seven European stations. The top-down fluxes of biogenic, pyrogenic, and anthropogenic VOC sources are optimized using an inversion framework based on the MAGRITTEv1.1 chemistry transport model and its adjoint. The inversion leads to strongly increased isoprene emissions with respect to the MEGAN-MOHYCAN inventory over the model domain (from 8.1 to 18.5 Tg yr−1 ) which is driven by the high observed TROPOMI HCHO columns in southern Europe. The impact of the inversion on biomass burning VOCs (+13%) and anthropogenic VOCs (−17%) is moderate. An evaluation of the optimized HCHO distribution against ground-based remote sensing (FTIR and MAX-DOAS) and in situ data provides generally improved agreement at stations below about 50° N, but indicates overestimated emissions in northern Scandinavia. Sensitivity inversions show that the top-down emissions are robust with respect to changes in the inversion settings and in the model chemical mechanism. However, the top-down emissions are very sensitive to the bias correction of the observed columns. Furthermore, the use of different a priori emissions has a significant impact on the inversion results due to large differences among bottom-up inventories. In regions with variable meteorology, there is strong week-to-week variability in the observed HCHO columns. The top-down emissions, which are optimized at weekly increments, have a much improved capability of representing these large fluctuations than an inversion using monthly increments. [ABSTRACT FROM AUTHOR]

The Geostationary Environment Monitoring Spectrometer (GEMS) onboard GEO-KOMPSAT 2B was successfully launched in February 2020 and has monitored Asia. We present the first evaluation of the operational GEMS formaldehyde (HCHO) vertical column densities (VCDs) during the in-orbit test period (IOT) (August–October 2020) and onward by comparing them with the products from Tropospheric Monitoring Instrument (TROPOMI), Fourier-Transform Infrared (FTIR), and Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) instruments. During the in-orbit test period, the GEMS HCHO VCDs reproduced the observed spatial pattern of TROPOMI VCDs over the whole domain (r=0.62) with high biases (10–16 %). In the afternoon, GEMS VCDs were too high over the west side of the tropics. We corrected this issue by adding polarization sensitivity vectors of the GEMS instrument as an additional fitting parameter in the retrieval algorithm. Using observed radiances from clear-sky pixels as the reference spectrum in the spectral fitting significantly contributed to reducing artifacts in radiance references, resulting in 10–40 % lower HCHO VCDs over the latitude including cloudy areas in the updated GEMS product. We find that the agreement between the two is much higher in Northeast Asia (r=0.90), including the Korean peninsula and East China. GEMS HCHO VCDs well captured the seasonal variation of HCHO mainly driven by biogenic emissions and photochemical activities but showed larger variations than those of TROPOMI over coastal regions (Kuala Lumpur, Singapore, Shanghai, and Busan). In addition, GEMS HCHO VCDs showed consistent hourly variations with MAX-DOAS (r=0.79) and FTIR (r=0.85) but were lower by 30–40 % relative to the ground based observations. Different vertical sensitivities between GEMS and ground-based instruments caused these systematic biases. The use of averaging kernel smoothing method reduces the low biases by about 10 to 15 % (NMB: -48.5 % to -32.4 %, -39.1 % to -27.3 % for MAX-DOAS and FTIR, respectively). The remaining discrepancies are due to multiple factors, including spatial colocation and different instrumental sensitivities, which need further investigation using inter-comparable datasets. [ABSTRACT FROM AUTHOR]