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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]

Instruments for air quality observations on geostationary satellites provide multiple observations per day and allow for the analysis of the diurnal variation of important air pollutants such as nitrogen dioxide (NO2) over large areas. The South Korean instrument GEMS on the GK2B satellite was launched in February 2020 and is the first instrument in geostationary orbit that delivers hourly daytime observations of NO2. The measurements with a spatial resolution of 3.5 km x 8 km cover a large part of Asia. This study compares one year of tropospheric NO2 vertical column density (VCD) observations of the operational GEMS L2 product, the scientific GEMS IUP-UB product, the operational TROPOMI product, and ground-based DOAS measurements in South Korea. The GEMS L2 tropospheric NO2 VCDs overestimate the VCDs retrieved from the ground-based observations with a median relative difference of +64 % and a correlation coefficient of 0.75. The median relative difference is -1 % for the GEMS IUP-UB product and -14 % for the TROPOMI product. The evaluation of the GEMS IUP-UB product and the operational TROPOMI product with ground-based measurements is in good agreement with correlation coefficients of 0.82 and 0.88. The scatter in the GEMS products can be reduced when observations are limited to the TROPOMI overpass time. The observed diurnal variations of the tropospheric NO2 VCDs show a maximum of NO2 during the late morning for urban sites, whereas rural sites show weak or almost no diurnal changes. Investigations of the seasonal diurnal variability show with a minimum in the observed tropospheric NO2 VCDs around noon the importance of chemical loss of NO2 in summer. Most variability is seen in spring and autumn, which dominate the average annual diurnal cycle. Observations under low wind conditions show strong enhancements of NO2 over the day, especially at polluted sites during winter. This indicates that under calm conditions, dilution and the less effective chemical loss in winter do not balance the accumulating emissions. The impact of transport processes is illustrated by the diurnal variability at a rural site following mean wind patterns for specific seasons and observation times. Analyzing the weekday-weekend effect, good agreement was found between the different products. However, the GEMS L2 product while agreeing with the other data sets during weekdays shows significantly less reduction on weekends. Our investigations show that the observed diurnal evolution of NO2 varies significantly at the different measurement sites, with good agreement between the GEMS IUP-UB and ground-based observations. The diurnal variability of tropospheric NO2 VCDs depends on chemistry, emissions, and transport into and out of the measurement region. To interpret the sources and sinks of NO2 requires that all of these factors are considered. [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]

We use formaldehyde (HCHO) vertical column measurements from the Scanning Imaging Absorption spectrometer for Atmospheric Chartography (SCIAMACHY) and Ozone Monitoring Instrument (OMI), and a nested-grid version of the GEOS-Chem chemistry transport model, to infer an ensemble of top-down isoprene emission estimates from tropical South America during 2006, using different model configurations and assumptions in the HCHO air-mass factor (AMF) calculation. Scenes affected by biomass burning are removed on a daily basis using fire count observations, and we use the local model sensitivity to identify locations where the impact of spatial smearing is small, though this comprises spatial coverage over the region. We find that the use of the HCHO column data more tightly constrains the ensemble isoprene emission range from 27-61 Tg C to 31-38 Tg C for SCIAMACHY, and 45-104 Tg C to 28-38 Tg C for OMI. Median uncertainties of the top-down emissions are about 60-260% for SCIAMACHY, and 10-90% for OMI. We find that the inferred emissions are most sensitive to uncertainties in cloud fraction and cloud top pressure (differences of ±10%), the a priori isoprene emissions (±20%), and the HCHO vertical column retrieval (±30%). Construction of continuous top-down emission maps generally improves GEOS-Chem's simulation of HCHO columns over the region, with respect to both the SCIAMACHY and OMI data. However, if local time top-down emissions are scaled to monthly mean values, the annual emission inferred from SCIAMACHY are nearly twice those from OMI. This difference cannot be explained by the different sampling of the sensors or uncertainties in the AMF calculation. Key Points Satellite HCHO data constrain range of uncertainty in Amazon isoprene emissions Top-down emissions are sensitive to prior isoprene inventory and HCHO retrieval Top-down emissions from SCIAMACHY are about twice those derived from OMI © 2013. American Geophysical Union. All Rights Reserved.

We use a nested-grid version of the GEOS-Chem chemistry transport model, constrained by isoprene emissions from the Model of Emissions of Gases and Aerosols from Nature (MEGAN), and the Lund-Potsdam-Jena General Ecosystem Simulator (LPJ-GUESS) bottom-up inventories, to evaluate the impact that surface isoprene emissions have on formaldehyde (HCHO) air-mass factors (AMFs) and vertical column densities (VCDs) over tropical South America during 2006, as observed by the Scanning Imaging Absorption Spectrometer for Atmospheric Chartography (SCIAMACHY) and Ozone Monitoring Instrument (OMI). Although the large-scale seasonal variability of monthly mean HCHO VCDs is typically unaffected by the choice of bottom-up inventory, large relative differences of up to ±45% in the HCHO VCD can occur for individual regions and months, but typically most VCD differences are of order ±20%. These relative changes are comparable to those produced by other sources of uncertainty in the AMF including aerosols and surface albedo, but less than those from clouds. In a sensitivity test, we find that top-down annual isoprene emissions inferred from SCIAMACHY and OMI HCHO vertical columns can vary by as much as ±30-50% for each instrument respectively, depending on the region studied and the a priori isoprene emissions used. Our analysis suggests that the influence of the a priori isoprene emissions on HCHO AMFs and VCDs is therefore non-negligible and must be carefully considered when inferring top-down isoprene emissions estimates over this, or potentially any other, region. © 2012. American Geophysical Union.

We present an evaluation of a nested high-resolution Goddard Earth Observing System (GEOS)-Chem chemistry transport model simulation of tropospheric chemistry over tropical South America. The model has been constrained with two isoprene emission inventories: (1) the canopy-scale Model of Emissions of Gases and Aerosols from Nature (MEGAN) and (2) a leaf-scale algorithm coupled to the Lund-Potsdam-Jena General Ecosystem Simulator (LPJ-GUESS) dynamic vegetation model, and the model has been run using two different chemical mechanisms that contain alternative treatments of isoprene photo-oxidation. Large differences of up to 100 Tg C yr-1 exist between the isoprene emissions predicted by each inventory, with MEGAN emissions generally higher. Based on our simulations we estimate that tropical South America (30-85°W, 14°N-25°S) contributes about 15-35% of total global isoprene emissions. We have quantified the model sensitivity to changes in isoprene emissions, chemistry, boundary layer mixing, and soil NOx emissions using ground-based and airborne observations. We find GEOS-Chem has difficulty reproducing several observed chemical species; typically hydroxyl concentrations are underestimated, whilst mixing ratios of isoprene and its oxidation products are overestimated. The magnitude of model formaldehyde (HCHO) columns are most sensitive to the choice of chemical mechanism and isoprene emission inventory. We find GEOS-Chem exhibits a significant positive bias (10-100%) when compared with HCHO columns from the Scanning Imaging Absorption Spectrometer for Atmospheric Chartography (SCIAMACHY) and Ozone Monitoring Instrument (OMI) for the study year 2006. Simulations that use the more detailed chemical mechanism and/or lowest isoprene emissions provide the best agreement to the satellite data, since they result in lower-HCHO columns. Copyright © 2011 by the American Geophysical Union.

We perform Empirical Orthogonal Function (EOF) analysis on 12 years of global GOME and SCIAMACHY formaldehyde (HCHO) column observations to determine the most significant spatial and temporal HCHO variations. In most regions, we find that HCHO variability is predominantly driven by seasonal variations of biogenie emissions and biomass burning. However, unusually low HCHO columns are consistently observed over the Amazon rainforest during the transition from the wet-to-dry seasons. We use MODIS leaf area and enhanced vegetation indices, to show variations in vegetation are consistent with the observed decrease in HCHO during this period (correlations of 0.69 and 0.67, respectively). Based on this evidence, we suggest isoprene emitting vegetation experience widespread leaf flushing (new leaf growth) prior to the dry season, resulting in a large-scale annual shutdown of Amazonian isoprene emissions. © 2009.

Bromine is a reactive trace element in the atmosphere, that destroys ozone, oxidizes mercury, modifies oxidative capacity and affects the lifetime of climate-active gases (e.g., methane). About 75 % of tropospheric ozone and methane is destroyed in the tropics, primarily in the lower free troposphere, where bromine monoxide (BrO) radical measurements are generally scarce. The few available aircraft observations find BrO is variable, and measurements in different compartments of the atmosphere are not easily reconciled. While zenith-sky DOAS measurements provide long-term records of the stratospheric O3 and NO2 abundances, autonomous MAX-DOAS placed at remote mountaintop observatories (MT-DOAS) provides cost effective and maximally sensitive access to probe the lower free troposphere, a climate-relevant yet understudied region of the atmosphere. Here we describe and evaluate an innovative full-atmosphere BrO and formaldehyde (HCHO) profile retrieval algorithm using MT-DOAS measurements at Mauna Loa Observatory (19.536° N; 155.577° W; 3401 m asl) during two case study days, characterized by the absence (26 Apr 2017, base case) and presence of a Rossby Wave breaking double tropopause (29 Apr 2017, RW-DT case) above Big Island, Hawaii. The full atmosphere retrieval is based on time-dependent optimal estimation, and simultaneously inverts 190+ individual BrO (and formaldehyde, HCHO) SCDs (slant column densities, SCD = dSCD + SCDRef) from solar stray light spectra measured in the zenith and off-axis geometries at high and low solar zenith angle (92º > SZA > 30º) to derive BrO concentration profiles with 7.5 degrees of freedom (DoF) from 1.9 to 35 km altitude. Stratospheric BrO vertical columns are near identical on both days (VCD = (1.5 ± 0.2) ×1013 molec cm-2), and the stratospheric BrO profile peaks at a lower altitude during the Rossby wave breaking event (1.6 – 2.0 DoFs). Tropospheric BrO VCDs increase from (0.70 ± 0.14) ×1013 molec cm-2 (base case) to (1.00 ± 0.14) ×1013 molec cm-2 (RW-DT), owing to a tropospheric BrO profile re-distribution characterized by a three-fold increase in BrO located in the upper troposphere (1.7 – 1.9 DoF). BrO is found to be more variable in the lower free troposphere (0.2 pptv < BrO < 0.9 pptv) and characterized in three altitude layers (near, above, below) MLO with added time resolution (~3.8 DoF). The BrO mixing ratio at MLO increases from (0.23 ± 0.03) pptv (base case) to (0.46 ± 0.03) pptv BrO (RW-DT); while the maximum of (0.9 ± 0.1) pptv BrO is observed above MLO in the lower free troposphere in absence of the double tropopause. We validate the retrieval using aircraft BrO profiles and in-situ HCHO measurements aboard the NSF/NCAR GV aircraft above MLO (11 Jan 2014) that establish BrO peaks around 2.4 pptv above 13 km in the UTLS during a similar RW-DT event (0.83 ×1013 molec cm-2 tropospheric BrO VCD above 2 km). The tropospheric BrO profile measured from MT-DOAS (RW-DT case) and the aircraft agree well (after averaging kernel smoothing). Furthermore, these tropospheric BrO profiles over the Central Pacific are found to closely resemble those over the Eastern Pacific Ocean (2–14 km); and contrast with the Western Pacific Ocean, where a C-shaped tropospheric BrO profile shape had been observed. [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]