HCHO Vertical Column Densities Research Articles

Interannual variability of summertime formaldehyde (HCHO) vertical column density and its main drivers at northern high latitudes

Abstract. The northern high latitudes (50–90° N, mostly including boreal-forest and tundra ecosystems) have been undergoing rapid climate and ecological changes over recent decades, leading to significant variations in volatile organic compounds (VOC) emissions from biogenic and biomass burning sources. Formaldehyde (HCHO) is an indicator of VOC emissions, but the interannual variability of HCHO and its main drivers over the region remains unclear. In this study, we use the GEOS-Chem chemical transport model and satellite retrievals from the Ozone Monitoring Instrument (OMI) and the Ozone Mapping and Profiler Suite (OMPS) to examine the interannual variability of HCHO vertical column density (VCD) during the summer seasons spanning from 2005 to 2019. Our results show that, in 2005–2019 summers, wildfires contributed 75 %–90 % of the interannual variability of HCHO VCD over Siberia, Alaska and northern Canada, while biogenic emissions and background methane oxidation account for ∼ 90 % of HCHO interannual variability over eastern Europe. We find that monthly solar-induced chlorophyll fluorescence (SIF) from the Orbiting Carbon Observatory-2 (OCO-2), an efficient proxy for plant photosynthesis, shows a good linear relationship (R= 0.6–0.7) with the modeled biogenic HCHO column (dVCDBio,GC) in eastern Europe, Siberia, Alaska and northern Canada, indicating the coupling between SIF and biogenic VOC emissions over the four domains on a monthly scale. In Alaska, Siberia and northern Canada, SIF and dVCDBio,GC both show relatively lower interannual variabilities (SIF: CV = 1 %–9 %, dVCDBio,GC: CV = 1 %–2 %; note that CV stands for coefficient of variation) in comparison to wildfire-induced HCHO (CV = 8 %–13 %), suggesting that the high interannual variabilities of OMI HCHO VCD (CV = 10 %–16 %) in these domains are likely driven by wildfires instead of biogenic emissions.

Unexpected HCHO transnational transport: influence on the temporal and spatial distribution of HCHO in Tibet from 2013 to 2021 based on satellite

Formaldehyde (HCHO) is a serious hazardous air pollutant and crucial precursor of PM2.5 and ozone compound pollution. There has been a dearth of HCHO research in Tibet where pressing need to protect the unique ecosystem. Therefore, this study aims to investigate the spatial-temporal distribution of HCHO from 2013 to 2021 and identify its influencing factors using satellite observations. Our findings reveal a noteworthy annual growth rate of 2.25% yr−1 in HCHO vertical column density (VCD) in Tibet. This rate is comparable to that in India and even surpasses levels observed in many other regions worldwide, including eastern China. Furthermore, unlike other areas, the eastern region of Tibet exhibits no discernible seasonal pattern in HCHO VCD. The anomalous variation in HCHO concentrations in Tibet can primarily be attributed to long-distance transnational transport originating from incomplete combustion in India Assam. Our research underscores the urgent need for enhanced atmospheric environmental management in Tibet.

Validation of OMPS Suomi NPP and OMPS NOAA‐20 Formaldehyde Total Columns With NDACC FTIR Observations

AbstractWe validate formaldehyde (HCHO) vertical column densities (VCDs) from Ozone Mapping and Profiler Suite Nadir Mapper (OMPS‐NM) instruments onboard the Suomi National Polar‐orbiting Partnership (Suomi NPP) satellite for 2012–2020 and National Oceanic and Atmospheric Administration‐20 (NOAA‐20) satellite for 2018–2020, hereafter referred to as OMPS‐NPP and OMPS‐N20, with ground‐based Fourier‐Transform Infrared (FTIR) observations of the Network for the Detection of Atmospheric Composition Change (NDACC). OMPS‐NPP/N20 HCHO products reproduce seasonal variability at 24 FTIR sites. Monthly variability of OMPS‐NPP/N20 has a very good agreement with FTIR, showing correlation coefficients of 0.83 and 0.88, respectively. OMPS‐NPP (N20) biases averaged over all sites are −0.9 (4) ± 3 (6)%. However, at clean sites (with VCDs < 4.0 × 1015 molecules cm−2), positive biases of 20 (32) ± 6 (18)% occur for OMPS‐NPP (N20). At sites with HCHO VCDs > 4.0 × 1015 molecules cm−2, negative biases of −15% ± 4% appear for OMPS‐NPP, but OMPS‐N20 shows smaller bias of 0.5% ± 6% due to its smaller ground pixel footprints. Therefore, smaller satellite footprint sizes are important in distinguishing small‐scale plumes. In addition, we discuss a bias correction and provide lower limit for the monthly uncertainty of OMPS‐NPP/N20 HCHO products. The total uncertainty for OMPS‐NPP (N20) at clean sites is 0.7 (0.8) × 1015 molecules cm−2, corresponding to a relative uncertainty of 32 (30)%. In the case of HCHO VCDs > 4.0 × 1015 molecules cm−2, however, the relative uncertainty in HCHO VCDs for OMPS‐NPP (N20) decreases to 31 (18)%.

Mobile MAX-DOAS observations of tropospheric NO2 and HCHO during summer over the Three Rivers' Source region in China

Abstract. The tropospheric concentrations of nitrogen dioxide (NO2) and formaldehyde (HCHO) have high spatio-temporal variability, and in situ observations of these trace gases are still scarce, especially in remote background areas. We made four similar circling journeys of mobile multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements in the Three Rivers' Source region over the Tibetan Plateau in summer (18–30 July) 2021 for the first time. The differential slant column densities (DSCDs) of NO2 and HCHO were retrieved from the measured spectra, with very weak absorptions along the driving routes. The tropospheric NO2 and HCHO vertical column densities (VCDs) were calculated from their DSCDs by the geometric approximation method, and they were further filtered to form reliable data sets by eliminating the influences of sunlight shelters and the vehicle's vibration and bumpiness. The observational data show that the tropospheric NO2 and HCHO VCDs decreased with the increasing altitude of the driving route, whose background levels ± standard deviations were 0.40 ± 1.13×1015 molec. cm−2 for NO2 and 2.27±1.66×1015 molec. cm−2 for HCHO in July 2021 over the Three Rivers' Source region. The NO2 VCDs show similar geographical distribution patterns between the different circling journeys, but the levels of the HCHO VCDs are different between the different circling journeys. The elevated NO2 VCDs along the driving routes usually corresponded to enhanced transport emissions from the towns crossed. However, the spatial distributions of the HCHO VCDs depended significantly on natural and meteorological conditions, such as surface temperature. By comparing TROPOMI satellite products and mobile MAX-DOAS results, we found that TROPOMI NO2 and HCHO VCDs have large positive offsets in the background atmosphere over the main area of the Three Rivers' Source. Our study provides valuable data sets and information of NO2 and HCHO over the Tibetan Plateau, benefitting the scientific community in investigating the spatio-temporal evolution of atmospheric composition in the background atmosphere at high altitudes, validating and improving the satellite products over mountain terrains, and evaluating the model's ability to simulate atmospheric chemistry over the Tibetan Plateau.

Source and variability of formaldehyde (HCHO) at northern high latitudes: an integrated satellite, aircraft, and model study

Abstract. Here we use satellite observations of formaldehyde (HCHO) vertical column densities (VCD) from the TROPOspheric Monitoring Instrument (TROPOMI), aircraft measurements, combined with a nested regional chemical transport model (GEOS-Chem at 0.5×0.625∘ resolution), to better understand the variability and sources of summertime HCHO in Alaska. We first evaluate GEOS-Chem with in-situ airborne measurements during the Atmospheric Tomography Mission 1 (ATom-1) aircraft campaign. We show reasonable agreement between observed and modeled HCHO, isoprene, monoterpenes and the sum of methyl vinyl ketone and methacrolein (MVK+MACR) in the continental boundary layer. In particular, HCHO profiles show spatial homogeneity in Alaska, suggesting a minor contribution of biogenic emissions to HCHO VCD. We further examine the TROPOMI HCHO product in Alaska in summer, reprocessed by GEOS-Chem model output for a priori profiles and shape factors. For years with low wildfire activity (e.g., 2018), we find that HCHO VCDs are largely dominated by background HCHO (58 %–71 %), with minor contributions from wildfires (20 %–32 %) and biogenic VOC emissions (8 %–10 %). For years with intense wildfires (e.g., 2019), summertime HCHO VCD is dominated by wildfire emissions (50 %–72 %), with minor contributions from background (22 %–41 %) and biogenic VOCs (6 %–10 %). In particular, the model indicates a major contribution of wildfires from direct emissions of HCHO, instead of secondary production of HCHO from oxidation of larger VOCs. We find that the column contributed by biogenic VOC is often small and below the TROPOMI detection limit, in part due to the slow HCHO production from isoprene oxidation under low NOx conditions. This work highlights challenges for quantifying HCHO and its precursors in remote pristine regions.

Ground-Based MAX-DOAS Measurements of Tropospheric Aerosols, NO2, and HCHO Distributions in the Urban Environment of Shanghai, China

Aerosol extinction profiles at 550 nm were retrieved by applying multi-axis differential optical absorption spectroscopy (MAX-DOAS) and lookup table. Then the tropospheric NO2 and HCHO vertical column densities were retrieved using a two-step method from 28 July to 5 August of 2015 in Shanghai. The retrieved results were compared with the satellite products, and then their diurnal variation was observed. A consistency check was performed before the inversion to obtain a correction factor. Based on the sensitivity of geometric angles to oxygen dimer air mass factor (O4 AMF, AMF is the ratio of the slanted column density to the vertical column density), the parameterization scheme of geometric angles in the lookup table is optimized. The results show that the aerosol increased significantly in the afternoon. The diurnal variation of tropospheric NO2 and HCHO vertical column densities (VCDs) are bimodal and unimodal patterns respectively, and their values are higher than those of GOME-2 and OMI satellite products. A process of aerosol reduction and recovery are related to ground particulates and meteorological elements. The chemical sensitivity of local ozone production also has a clear diurnal variation.

Identification of ozone sensitivity for NO2 and secondary HCHO based on MAX-DOAS measurements in northeast China.

In this study, tropospheric formaldehyde (HCHO) vertical column densities (VCDs) were measured using multi-axis differential optical absorption spectroscopy (MAX-DOAS) from January to November 2019 in Shenyang, Northeast China. The maximum HCHO VCD value appeared in the summer (1.74×1016 molec/cm2), due to increased photo-oxidation of volatile organic compounds (VOCs). HCHO concentrations increased from 08:00 and peaked near 13:00, which was mainly attributed to the increased release of isoprene from plants and enhanced photolysis at noon. The HCHO VCDs observed by MAX-DOAS and OMI have a good correlation coefficient (R) of 0.78, and the contributions from primary and secondary HCHO sources were distinguished by the multi-linear regression model. The anthropogenic emissions showed unobvious seasonal variations, and the primary HCHO was relatively stable in Shenyang. Secondary HCHO contributed 82.62%, 83.90%, 78.90%, and 41.53% to the total measured ambient HCHO during the winter, spring, summer, and autumn, respectively. We also found a good correlation (R=0.78) between enhanced vegetation index (EVI) and HCHO VCDs, indicating that the oxidation of biogenic volatile organic compounds (BVOCs) was the main source of HCHO. The ratio of secondary HCHO to nitrogen dioxide (NO2) was used as the tracer to analyze O3-NOx-VOC sensitivities. We found that the VOC-limited, VOC-NOx-limited, and NOx-limited regimes made up 93.67%, 6.23%, 0.11% of the overall measurements, respectively. In addition, summertime ozone (O3) sensitivity changed from VOC-limited in the morning to VOC-NOx-limited in the afternoon. Therefore, this study offers information on HCHO sources and corresponding O3 production sensitivities to support strategic management decisions.

First global observation of tropospheric formaldehyde from Chinese GaoFen-5 satellite: Locating source of volatile organic compounds

Satellite remote sensing is an important technique providing long-term and large-scale information of formaldehyde (HCHO), which plays a crucial role in atmospheric chemistry. Low signal-to-noise ratio and poor stability of the Environmental Trace Gases Monitoring Instrument (EMI) On board Gaofen-5 satellite, the first Chinese space-borne spectrometer, make HCHO retrieval extremely difficult. Here we firstly retrieved HCHO vertical column densities (VCDs) from EMI through in-flight spectral calibration, retrieval setting optimization and stripe correction. Retrieved EMI HCHO VCDs correlate well with those measured by Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) with normalize mean bias (NMB) below 25%. EMI HCHO VCDs are comparable with those observed by Ozone Monitoring Instrument (OMI) and TROPOspheric Monitoring Instrument (TROPOMI). This study reveals that HCHO can be observed successfully by algorithm optimization despite of poor performance of space-borne spectrometer. The retrieved EMI HCHO VCDs are applied to locate emission sources of volatile organic compounds (VOCs).

OMI-observed HCHO in Shanghai, China, during 2010–2019 and ozone sensitivity inferred by an improved HCHO ∕ NO2 ratio

Abstract. In recent years, satellite remote sensing has been increasingly used in the long-term observation of ozone (O3) precursors and its formation regime. In this work, formaldehyde (HCHO) data from Ozone Monitoring Instrument (OMI) were used to analyze the temporal and spatial distribution of HCHO vertical column densities (VCDs) in Shanghai from 2010 to 2019. HCHO VCDs exhibited the highest value in summer and the lowest in winter, the high VCD being concentrated in western Shanghai. Temperature largely influences HCHO by affecting the biogenic emissions and photochemical reactions, and industry was the major anthropogenic source. The satellite-observed formaldehyde-to-nitrogen dioxide ratio (FNRSAT) reflects that the O3 formation regime had significant seasonal characteristics and gradually manifested as a transitional ozone formation regime dominating in Shanghai. The uneven distribution in space was mainly reflected in the higher FNRSAT and surface O3 concentration in suburban areas. To compensate for the shortcoming of FNRSAT that it can only characterize O3 formation around satellite overpass time, correction of FNRSAT was implemented with hourly surface FNR and O3 data. After correction, the O3 formation regime showed the trend moving towards being VOC-limited in both time and space, and the regime indicated by FNRSAT can better reflect O3 formation for a day. This study can help us better understand HCHO characteristics and O3 formation regimes in Shanghai and also provide a method to improve FNRSAT for characterizing O3 formation in a day, which will be significant for developing O3 prevention and control strategies.

Global Surface HCHO Distribution Derived from Satellite Observations with Neural Networks Technique

Formaldehyde (HCHO) is one of the most important carcinogenic air contaminants in outdoor air. However, the lack of monitoring of the global surface concentration of HCHO is currently hindering research on outdoor HCHO pollution. Traditional methods are either restricted to small areas or, for research on a global scale, too data-demanding. To alleviate this issue, we adopted neural networks to estimate the 2019 global surface HCHO concentration with confidence intervals, utilizing HCHO vertical column density data from TROPOMI, and in-situ data from HAPs (harmful air pollutants) monitoring networks and the ATom mission. Our results show that the global surface HCHO average concentration is 2.30 μg/m3. Furthermore, in terms of regions, the concentrations in the Amazon Basin, Northern China, South-east Asia, the Bay of Bengal, and Central and Western Africa are among the highest. The results from our study provide the first dataset on global surface HCHO concentration. In addition, the derived confidence intervals of surface HCHO concentration add an extra layer of confidence to our results. As a pioneering work in adopting confidence interval estimation to AI-driven atmospheric pollutant research and the first global HCHO surface distribution dataset, our paper paves the way for rigorous study of global ambient HCHO health risk and economic loss, thus providing a basis for pollution control policies worldwide.

Top-down estimates of anthropogenic VOC emissions in South Korea using formaldehyde vertical column densities from aircraft during the KORUS-AQ campaign

Nonmethane volatile organic compounds (NMVOCs) result in ozone and aerosol production that adversely affects the environment and human health. For modeling purposes, anthropogenic NMVOC emissions have been typically compiled using the “bottom-up” approach. To minimize uncertainties of the bottom-up emission inventory, “top-down” NMVOC emissions can be estimated using formaldehyde (HCHO) observations. In this study, HCHO vertical column densities (VCDs) obtained from the Geostationary Trace gas and Aerosol Sensor Optimization spectrometer during the Korea–United States Air Quality campaign were used to constrain anthropogenic volatile organic compound (AVOC) emissions in South Korea. Estimated top-down AVOC emissions differed from those of the up-to-date bottom-up inventory over major anthropogenic source regions by factors of 1.0 ± 0.4 to 6.9 ± 3.9. Our evaluation using a 3D chemical transport model indicates that simulated HCHO mixing ratios using the top-down estimates were in better agreement with observations onboard the DC-8 aircraft during the campaign relative to those with the bottom-up emission, showing a decrease in model bias from –25% to –13%. The top-down analysis used in this study, however, has some limitations related to the use of HCHO yields, background HCHO columns, and AVOC speciation in the bottom-up inventory, resulting in uncertainties in the AVOC emission estimates. Our attempt to constrain diurnal variations of the AVOC emissions using the aircraft HCHO VCDs was compromised by infrequent aircraft observations over the same source regions. These limitations can be overcome with geostationary satellite observations by providing hourly HCHO VCDs.

Formaldehyde total column densities over Mexico City: comparison between multi-axis differential optical absorption spectroscopy and solar-absorption Fourier transform infrared measurements

Abstract. Formaldehyde (HCHO) total column densities over the Mexico City metropolitan area (MCMA) were retrieved using two independent measurement techniques: multi-axis differential optical absorption spectroscopy (MAX-DOAS) and Fourier transform infrared (FTIR) spectroscopy. For the MAX-DOAS measurements, the software QDOAS was used to calculate differential slant column densities (dSCDs) from the measured spectra and subsequently the Mexican MAX-DOAS fit (MMF) retrieval code to convert from dSCDs to vertical column densities (VCDs). The direct solar-absorption spectra measured with FTIR were analyzed using the PROFFIT (PROFile FIT) retrieval code. Typically the MAX-DOAS instrument reports higher VCDs than those measured with FTIR, in part due to differences found in the ground-level sensitivities as revealed from the retrieval diagnostics from both instruments, as the FTIR and the MAX-DOAS information do not refer exactly to the same altitudes of the atmosphere. Three MAX-DOAS datasets using measurements conducted towards the east, west or both sides of the measurement plane were evaluated with respect to the FTIR results. The retrieved MAX-DOAS HCHO VCDs where 6 %, 8 % and 28 % larger than the FTIR measurements which, supported with satellite data, indicates a large horizontal inhomogeneity in the HCHO abundances. The temporal change in the vertical distribution of this pollutant, guided by the evolution of the mixing-layer height, affects the comparison of the two retrievals with different sensitivities (total column averaging kernels). In addition to the reported seasonal and diurnal variability of HCHO columns within the urban site, background data from measurements at a high-altitude station, located only 60 km away, are presented.

Long-term MAX-DOAS measurements of NO<sub>2</sub>, HCHO, and aerosols and evaluation of corresponding satellite data products over Mohali in the Indo-Gangetic Plain

Abstract. We present comprehensive long-term ground-based multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements of aerosols, nitrogen dioxide (NO2), and formaldehyde (HCHO) from Mohali (30.667∘ N, 76.739∘ E; ∼310 m above mean sea level), located in the densely populated Indo-Gangetic Plain (IGP) of India. We investigate the temporal variation in tropospheric columns, surface volume mixing ratio (VMR), and vertical profiles of aerosols, NO2, and HCHO and identify factors driving their ambient levels and distributions for the period from January 2013 to June 2017. We observed mean aerosol optical depth (AOD) at 360 nm, tropospheric NO2 vertical column density (VCD), and tropospheric HCHO VCD for the measurement period to be 0.63 ± 0.51, (6.7 ± 4.1) × 1015, and (12.1 ± 7.5) × 1015 molecules cm−2, respectively. Concerning the tropospheric NO2 VCDs, Mohali was found to be less polluted than urban and suburban locations of China and western countries, but comparable HCHO VCDs were observed. For the more than 4 years of measurements during which the region around the measurement location underwent significant urban development, we did not observe obvious annual trends in AOD, NO2, and HCHO. High tropospheric NO2 VCDs were observed in periods with enhanced biomass and biofuel combustion (e.g. agricultural residue burning and domestic burning for heating). Highest tropospheric HCHO VCDs were observed in agricultural residue burning periods with favourable meteorological conditions for photochemical formation, which in previous studies have shown an implication for high ambient ozone also over the IGP. Highest AOD is observed in the monsoon season, indicating possible hygroscopic growth of the aerosol particles. Most of the NO2 is located close to the surface, whereas significant HCHO is present at higher altitudes up to 600 m during summer indicating active photochemistry at high altitudes. The vertical distribution of aerosol, NO2, and HCHO follows the change in boundary layer height (BLH), from the ERA5 dataset of European Centre for Medium-Range Weather Forecasts, between summer and winter. However, deep convection during the monsoon transports the pollutants at high altitudes similar to summer despite a shallow ERA5 BLH. Strong gradients in the vertical profiles of HCHO are observed during the months when primary anthropogenic sources dominate the formaldehyde production. High-resolution MODIS AOD measurements correlate well but were systematically higher than MAX-DOAS AODs. The ground-based MAX-DOAS measurements were used to evaluate three NO2 data products and two HCHO data products of the Ozone Monitoring Instrument (OMI) for the first time over India and the IGP. NO2 VCDs from OMI correlate reasonably with MAX-DOAS VCDs but are lower by ∼30 %–50 % due to the difference in vertical sensitivities and the rather large OMI footprint. OMI HCHO VCDs exceed the MAX-DOAS VCDs by up to 30 %. We show that there is significant scope for improvement in the a priori vertical profiles of trace gases, which are used in OMI retrievals. The difference in vertical representativeness was found to be crucial for the observed biases in NO2 and HCHO surface VMR intercomparisons. Using the ratio of NO2 and HCHO VCDs measured from MAX-DOAS, we have found that the peak daytime ozone production regime is sensitive to both NOx and VOCs in winter but strongly sensitive to NOx in other seasons.

An improved TROPOMI tropospheric HCHO retrieval over China

Abstract. We present an improved TROPOspheric Monitoring Instrument (TROPOMI) retrieval of formaldehyde (HCHO) over China. The new retrieval optimizes the slant column density (SCD) retrieval and air mass factor (AMF) calculation for TROPOMI observations of HCHO over China. Retrieval of HCHO differential SCDs (DSCDs) is improved using the basic optical differential spectroscopy (BOAS) technique resulting in lower noise and smaller random error, while AMFs are improved with a priori HCHO profiles from a higher resolution regional chemistry transport model. Compared to the operational product, the new TROPOMI HCHO retrieval shows better agreement with ground-based Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) measurements in Beijing. The improvements are mainly related to the AMF calculation with more precise a priori profiles in winter. Using more precise a priori profiles in general reduces HCHO vertical column densities (VCDs) by 52.37 % (± 27.09 %) in winter. Considering the aerosol effect in AMF calculation reduces the operational product by 11.46 % (± 1.48 %) and our retrieval by 17.61 % (± 1.92 %) in winter. The improved and operational HCHO are also used to investigate the spatial–temporal characteristics of HCHO over China. The result shows that both improved and operational HCHO VCDs reach maximum in summer and minimum in winter. High HCHO VCDs mainly located over populated areas, i.e., Sichuan Basin and central and eastern China, indicate a significant contribution of anthropogenic emissions. The hotspots are more obvious on the map of the improved HCHO retrieval than the operational product. The result indicates that the improved TROPOMI HCHO retrieval is more suitable for the analysis of regional- and city-scale pollution in China.

Unexpected long-range transport of glyoxal and formaldehyde observed from the Copernicus Sentinel-5 Precursor satellite during the 2018 Canadian wildfires

Abstract. Glyoxal (CHOCHO) and formaldehyde (HCHO) are intermediate products in the tropospheric oxidation of the majority of volatile organic compounds (VOCs). CHOCHO is also a precursor of secondary organic aerosol (SOA) in the atmosphere. CHOCHO and HCHO are released from biogenic, anthropogenic, and pyrogenic sources. CHOCHO and HCHO tropospheric lifetimes are typically considered to be short during the daytime at mid-latitudes (e.g. several hours), as they are rapidly removed from the atmosphere by their photolysis, oxidation by OH, and uptake on particles or deposition. At night and at high latitudes, tropospheric lifetimes increase to many hours or even days. Previous studies demonstrated that CHOCHO and HCHO vertical column densities (VCDs) are well retrieved from space-borne observations using differential optical absorption spectroscopy (DOAS). In this study, we present CHOCHO and HCHO VCDs retrieved from measurements by TROPOMI (TROPOspheric Monitoring Instrument), launched on the Sentinel-5 Precursor (S5P) platform in October 2017. We observe strongly elevated amounts of CHOCHO and HCHO during the 2018 fire season in British Columbia, Canada, where a large number of fires occurred in August. CHOCHO and HCHO plumes from individual fire hot spots are observed in air masses travelling over distances of up to 1500 km, i.e. much longer than expected for the relatively short tropospheric lifetime expected for CHOCHO and HCHO. Comparison with simulations by the particle dispersion model FLEXPART (FLEXible PARTicle dispersion model) indicates that effective lifetimes of 20 h and more are needed to explain the observations of CHOCHO and HCHO if they decay in an effective first-order process. FLEXPART used in the study calculates accurately the transport. In addition an exponential decay, in our case assumed to be photochemical, of a species along the trajectory is added. We have used this simple approach to test our assumption that CHOCHO and HCHO are created in the fires and then decay at a constant rate in the plume as it is transported. This is clearly not the case and we infer that CHOCHO and HCHO are either efficiently recycled during transport or continuously formed from the oxidation of longer-lived precursors present in the plume, or possibly a mixture of both. We consider the best explanation of the observed CHOCHO and HCHO VCD in the plumes of the fire is that they are produced by oxidation of longer-lived precursors, which were also released by the fire and present in the plume.

Identifying the wintertime sources of volatile organic compounds (VOCs) from MAX-DOAS measured formaldehyde and glyoxal in Chongqing, southwest China

Ground-based multi-axis differential optical absorption spectroscopy (MAX-DOAS) observations were performed from 27 December 2018 to 16 January 2019 in Changshou, one of subdistricts of Chongqing, China. Primary atmospheric pollutant in Changshou during wintertime was PM2.5, whose contribution averaged about 70.15% ± 9.5% of PM10. The ratio of PM2.5/PM10 decreased when PM2.5 pollution became worse, and it should attribute to biomass burning and the contribution of hygroscopic growth and enhanced heterogeneous chemistry under high relative humidity condition. Moreover, nitrogen dioxide (NO2), formaldehyde (HCHO) and glyoxal (CHOCHO) vertical profiles during the campaign period were retrieved separately. TROPOMI HCHO vertical column densities (VCDs) and MAX-DOAS HCHO VCDs were correlated well (R = 0.93). In order to identify the sources of volatile organic compound (VOC) in Changshou, the ratio of CHOCHO to HCHO (RGF) in five different layers were estimated. The estimated daily averaged RGF were 0.0205 ± 0.0077, 0.0727 ± 0.0286, 0.0864 ± 0.0296, 0.0770 ± 0.0275 and 0.0746 ± 0.0263 in 0–100 m, 100–200 m, 300–400 m, 500–600 m and 700–800 m layers, respectively. The estimated RGF will increase when biomass burnings were dominated. Using NO2 as a tracer of anthropogenic emissions, we found the RGF values gradually decrease with the increase of NO2 levels. RGF values in 0–100 m layer and all the other upper layers are 0.015–0.025 and 0.06–0.14, and that means the dominant sources of VOCs in 0–100 m layer and all the other upper layers are biogenic emission and anthropogenic emission (especially biomass burning), respectively. In addition, we found that RGF has site dependence which is in compliance with several previous studies.

Explicit Aerosol Correction of OMI Formaldehyde Retrievals

Atmospheric aerosols are significant sources of uncertainty in air mass factor (AMF) calculations for trace gas retrievals using ultraviolet measurements from space. Current trace gas retrievals typically do not consider aerosols explicitly as cloud products partially account for aerosol effects. Here, we propose a new measurement‐based approach to correct for aerosols explicitly in the AMF calculation, apply it to Ozone Monitoring Instrument (OMI) formaldehyde (HCHO) retrievals and quantify the aerosol‐induced HCHO vertical column density difference for three aerosol types (smoke, dust, and sulfate) during 2006–2007. We use OMI aerosol retrievals for aerosol optical properties and vertical profiles to construct lookup tables of scattering weights as functions of geometry, surface pressure, surface albedo, and aerosol information. The average difference between the National Aeronautics and Space Administration operational OMI HCHO product (not considering aerosols) and the results obtained in this study on a global scale are 27%, 6%, and −0.3% for smoke, dust, and sulfate aerosols, respectively. The region with the largest aerosol effects is East China, where the explicit smoke aerosol correction enhances mean HCHO vertical column densities by 35%, with corrections to individual observations sometimes larger than 100%. The quantified aerosol effects are applicable under clear‐sky conditions. This study highlights the need to implement aerosol corrections in the AMF calculation for HCHO retrievals. This is particularly relevant in regions with high levels of pollution where aerosols interfere the most with formaldehyde satellite observations.

MAX-DOAS measurements of tropospheric NO<sub>2</sub> and HCHO in Nanjing and a comparison to ozone monitoring instrument observations

Abstract. In this paper, we present long-term observations of atmospheric nitrogen dioxide (NO2) and formaldehyde (HCHO) in Nanjing using a Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) instrument. Ground-based MAX-DOAS measurements were performed from April 2013 to February 2017. The MAX-DOAS measurements of NO2 and HCHO vertical column densities (VCDs) are used to validate ozone monitoring instrument (OMI) satellite observations over Nanjing. The comparison shows that the OMI observations of NO2 correlate well with the MAX-DOAS data with Pearson correlation coefficient (R) of 0.91. However, OMI observations are on average a factor of 3 lower than the MAX-DOAS measurements. Replacing the a priori NO2 profiles by the MAX-DOAS profiles in the OMI NO2 VCD retrieval would increase the OMI NO2 VCDs by ∼30 % with correlation nearly unchanged. The comparison result of MAX-DOAS and OMI observations of HCHO VCD shows a good agreement with R of 0.75 and the slope of the regression line is 0.99. An age-weighted backward-propagation approach is applied to the MAX-DOAS measurements of NO2 and HCHO to reconstruct the spatial distribution of NO2 and HCHO over the Yangtze River Delta during summer and winter time. The reconstructed NO2 fields show a distinct agreement with OMI satellite observations. However, due to the short atmospheric lifetime of HCHO, the backward-propagated HCHO data do not show a strong spatial correlation with the OMI HCHO observations. The result shows that the MAX-DOAS measurements are sensitive to the air pollution transportation in the Yangtze River Delta, indicating the air quality in Nanjing is significantly influenced by regional transportation of air pollutants. The MAX-DOAS data are also used to evaluate the effectiveness of air pollution control measures implemented during the Youth Olympic Games 2014. The MAX-DOAS data show a significant reduction of ambient aerosol, NO2 and HCHO (30 %–50 %) during the Youth Olympic Games. Our results provide a better understanding of the transportation and sources of pollutants over the Yangtze River Delta as well as the effect of emission control measures during large international events, which are important for the future design of air pollution control policies.

Estimation of HCHO Column Using a Multiple Regression Method with OMI and MODIS Data

We have estimated the vertical column density (VCD) of formaldehyde (HCHO) on a global scale using a multiple linear regression method (MRM) with Ozone Monitoring Instrument (OMI) and Moderate-Resolution Imaging Spectroradiometer (MODIS) data. HCHO VCDs were estimated in regions of biogenic, pyrogenic, and anthropogenic emissions using independent variables, including NO2 VCD, land surface temperature (LST), an enhanced vegetation index (EVI), and the mean fire radiative power (MFRP), which are strongly correlated with HCHO. To evaluate the HCHO estimates obtained using the MRM, we compared estimates of HCHO VCD data measured by OMI (HCHOOMI) with those estimated by multiple linear regression equations (MRE) (HCHOMRE). Good MRM performances were found, having the average statistical values (R = 0.91, slope = 1.03, mean bias = -0.12 × 1015 molecules cm-2, percent difference = 11.27%) between HCHOMRE and HCHOOMI in our study regions where high HCHO levels are present. Our results demonstrate that the MRM can be a useful tool for estimating atmospheric HCHO levels.

Ground ozone variations at an urban and a rural station in Beijing from 2006 to 2017: Trend, meteorological influences and formation regimes

Due to complicated ozone formation regimes controlled by both ozone precursors and meteorological conditions, the underlying drivers for soaring ozone concentrations in Beijing were limitedly examined. With ground observation and remotely sensed data, the variation of ground ozone concentrations at an urban AT (Aoti) station and a rural YF (Yufa) station in Beijing was examined and a notable upward trend of ozone concentrations at both stations was found from 2006 to 2017. Following this, through a statistical model, the relative contribution of meteorological conditions to long-term ozone variations at both stations was calculated as 2%–3%, indicating anthropogenic emissions were the major cause for long-term ozone variations in Beijing. Meanwhile, short-term ozone variations could be influenced significantly by seasonal and synoptic meteorological conditions. Furthermore, the long-term variations of ozone formation regimes across Beijing were analyzed using OMI (Ozone Monitoring Instrument) retrieved HCHO VCDs (Vertical Column Densities)/NO2 VCDs, which were strongly correlated with ozone concentrations. The results suggested that the ozone formation regime for the AT urban station and YF rural station had changed from VOCs-limited and NOx-limited to VOCs-NOx-limited respectively. In this case, NOx-oriented emission-reduction measures for reducing PM2.5 concentrations might conversely enhance ozone concentrations in Beijing. Given the increasingly heterogeneous distribution of different ozone formation regimes across Beijing, emission-reduction strategies that balanced consider the reduction of VOCs and NOx emissions should be better designed and implemented according to local ozone formation regimes.