HCHO Vertical Column Research Articles

The association between long-term exposure to ambient formaldehyde and respiratory mortality risk: A national study in China

IntroductionWhile ambient formaldehyde (HCHO) concentrations are increasing worldwide, there was limited research on its health effects. ObjectivesTo assess the association of long-term exposure to ambient HCHO with the risk of respiratory (RESP) mortality and the associated mortality burden in China. MethodsAnnual and seasonal RESP death and tropospheric HCHO vertical columns data were collected in 466 counties/districts across China during 2013–2016. A difference-in-differences approach combined with a generalized linear mixed-effects regression model was employed to assess the exposure-response association between long-term ambient HCHO exposure and RESP mortality risk. Additionally, we computed the attributable fraction (AF) to gauge the proportion of RESP mortality attributable to HCHO exposure. ResultsThis analysis encompassed 560,929 RESP deaths. The annual mean ambient HCHO concentration across selected counties/districts was 8.02×1015 ± 2.22×1015 molec.cm−2 during 2013–2016. Each 1.00×1015 molec.cm−2 increase in ambient HCHO was associated with a 1.61 % increase [excess risk (ER), 95 % confidence interval (CI): 1.20 %, 2.03 %] in the RESP mortality risk. The AF of RESP mortality attributable to HCHO was 12.16 % (95 %CI:9.33 %, 14.88 %), resulting in an annual average of 125,422 (95 %CI:96,404, 153,410) attributable deaths in China. Stratified analyses suggested stronger associations in individuals aged ≥65 years old (ER=1.87 %, 95 %CI:1.43 %, 2.32 %), in cold seasons (ER=1.00 %, 95 %CI:0.56 %, 1.44 %), in urban areas (ER=1.65 %, 95 %CI:1.15 %, 2.16 %), and in chronic obstructive pulmonary disease patients (ER=1.95 %, 95 %CI:1.42 %, 2.48 %). ConclusionsThis study suggested that long-term HCHO exposure may significantly increase the risk of RESP mortality, leading to a substantial mortality burden. Targeted measures should be implemented to control ambient HCHO pollution promptly.

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.

Global Formaldehyde Products From the Ozone Mapping and Profiler Suite (OMPS) Nadir Mappers on Suomi NPP and NOAA‐20

AbstractWe describe new publicly available, multi‐year formaldehyde (HCHO) data records from the Ozone Mapping and Profiler Suite (OMPS) nadir mapper (NM) instruments on the Suomi NPP and NOAA‐20 satellites. The OMPS‐NM instruments measure backscattered UV light over the globe once per day, with spatial resolutions close to nadir of 50 × 50 km2 (OMPS/Suomi‐NPP) and 17 × 17 km2 or 12 × 17 km2 (OMPS/NOAA‐20). After a preliminary instrument line shape and wavelength calibration using on‐orbit observations, we use the backscatter measurements in a direct spectral fit of radiances, in combination with a nadir reference spectrum collected over a clean area, to determine slant columns of HCHO. The slant columns are converted to vertical columns using air mass factors (AMFs) derived through scene‐by‐scene radiative transfer calculations. Finally, a correction is applied to account for background HCHO in the reference spectrum, as well as any remaining high‐latitude biases. We investigate the consistency of the OMPS products from Suomi NPP and NOAA‐20 using long‐term monthly means over 12 geographic regions, and also compare the products with publicly available TROPOMI HCHO observations. OMPS/Suomi‐NPP and OMPS/NOAA‐20 monthly mean HCHO vertical columns are highly consistent (r = 0.98), with low proportional (2%) and offset (2 × 1014 molecules cm−2) biases. OMPS HCHO monthly means are also well‐correlated with those from TROPOMI (r = 0.92), although they are consistently 10% ± 16% larger in polluted regions (columns >8 × 1015 molecules cm−2). These differences result primarily from differences in AMFs.

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.

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.

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.

Recommendations for HCHO and SO2 Retrieval Settings from MAX-DOAS Observations under Different Meteorological Conditions

Recently, the occurrence of fog and haze over China has increased. The retrieval of trace gases from the multi-axis differential optical absorption spectroscopy (MAX-DOAS) is challenging under these conditions. In this study, various reported retrieval settings for formaldehyde (HCHO) and sulfur dioxide (SO2) are compared to evaluate the performance of these settings under different meteorological conditions (clear day, haze, and fog). The dataset from 1st December 2019 to 31st March 2020 over Nanjing, China, is used in this study. The results indicated that for HCHO, the optimal settings were in the 324.5–359 nm wavelength window with a polynomial order of five. At these settings, the fitting and root mean squared (RMS) errors for column density were considerably improved for haze and fog conditions, and the differential slant column densities (DSCDs) showed more accurate values compared to the DSCDs between 336.5 and 359 nm. For SO2, the optimal settings for retrieval were found to be at 307–328 nm with a polynomial order of five. Here, root mean square (RMS) and fitting errors were significantly lower under all conditions. The observed HCHO and SO2 vertical column densities were significantly lower on fog days compared to clear days, reflecting a decreased chemical production of HCHO and aqueous phase oxidation of SO2 in fog droplets.

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.

A long-term estimation of biogenic volatile organic compound (BVOC) emission in China from 2001–2016: the roles of land cover change and climate variability

Abstract. Satellite observations reveal that China has been leading the global greening trend in the past 2 decades. We assessed the impact of land cover change as well as climate variability on total biogenic volatile organic compound (BVOC) emission in China from 2001–2016. We found the greening trend in China is leading a national-scale increase in BVOC emission. The BVOC emission level in 2016 could be 11.7 % higher than that in 2001 because of higher tree cover fraction and vegetation biomass. On the regional scale, the BVOC emission level from 2013–2016 could be 8.6 %–19.3 % higher than that from 2001–2004 in hotspots including (1) northeastern China, (2) Beijing and its surrounding areas, (3) the Qin Mountains, (4) Yunnan Province, (5) Guangxi–Guangdong provinces, and (6) Hainan island because of the land cover change without considering the impact of climate variability. The comparison among different scenarios showed that vegetation changes resulting from land cover management are the main driver of BVOC emission change in China. Climate variability contributed significantly to interannual variations but not much to the changing trend during the study period. In the standard scenario, which considers both land cover change and climate variability, a statistically significant increasing trend can still be found in regions including Beijing and its surroundings, Yunnan Province, and Hainan island, and BVOC emission total amount in these regions from 2013–2016 is 11.0 %–17.2 % higher that from 2001–2004. We compared the long-term HCHO vertical columns (VC) from the satellite-based Ozone Monitoring Instrument (OMI) with the estimation of isoprene emission in summer. The results showed statistically significant positive correlation coefficients over the regions with high vegetation cover fractions. In addition, the isoprene emission and HCHO VC both showed statistically significant increasing trends in the south of China where these two variables have high positive correlation coefficients. This result may support our estimation of the variability and trends of BVOC emission in this region; however, the comparison still has large uncertainties since the chemical and physical processes, including transportation, diffusion and chemical reactions, were not considered. Our results suggest that the continued increase in BVOC will enhance the importance of considering BVOC when making policies for controlling ozone pollution in China along with ongoing efforts to increase the forest cover fraction.

Comparison of formaldehyde tropospheric columns in Australia and New Zealand using MAX-DOAS, FTIR and TROPOMI

Abstract. South-eastern Australia has been identified by modelling studies as a hotspot of biogenic volatile organic compound (VOC) emissions; however, long-term observational VOC studies are lacking in this region. Here, 2.5 years of multi-axis differential optical absorption spectroscopy (MAX-DOAS) formaldehyde (HCHO) measurements in Australasia are presented, from Broadmeadows, in northern Melbourne, Australia, and from Lauder, a rural site in the South Island of New Zealand. Across the measurement period from December 2016 to November 2019, the mean formaldehyde columns measured by the MAX-DOAS were 2.50±0.61×1015 molec. cm−2 at Lauder and 5.40±1.59×1015 molec. cm−2 at Broadmeadows. In both locations, the seasonal cycle showed a pronounced peak in Austral summer (December–January–February) consistent with temperature-dependent formaldehyde production from biogenic precursor gases. The amplitude of the seasonal cycle was 0.7×1015 molec. cm−2 at Lauder, and it was 2.0×1015 molec. cm−2 at Broadmeadows. The Lauder MAX-DOAS HCHO measurements are compared with 27 months of co-located Fourier transform infrared (FTIR) observations. The seasonal variation of Lauder MAX-DOAS HCHO, smoothed by the FTIR averaging kernels, showed good agreement with the FTIR measurements, with a linear regression slope of 1.03 and an R2 of 0.66 for monthly averaged formaldehyde partial columns (0–4 km). In addition to ground-based observations, a clear way to address the VOC measurement gap in areas such as Australasia is with satellite measurements. Here, we demonstrate that the TROPOspheric Monitoring Instrument (TROPOMI) can be used to distinguish formaldehyde hotspots in forested and agricultural regions of south-eastern Australia. The MAX-DOAS measurements are also compared to TROPOMI HCHO vertical columns at Lauder and Melbourne; very strong monthly average agreement is found for Melbourne (regression slope of 0.61 and R2 of 0.95) and a strong agreement is found at Lauder (regression slope of 0.73 and R2 of 0.61) for MAX-DOAS vs. TROPOMI between May 2018 and November 2019. This study, the first long-term satellite comparison study using MAX-DOAS in the Southern Hemisphere, highlights the improvement offered by TROPOMI's high resolution over previous satellite products and provides the groundwork for future studies using ground-based and satellite DOAS for studying VOCs in Australasia.

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.

Description of a formaldehyde retrieval algorithm for the Geostationary Environment Monitoring Spectrometer (GEMS)

Abstract. We describe a formaldehyde (HCHO) retrieval algorithm for the Geostationary Environment Monitoring Spectrometer (GEMS) that will be launched by the Korean Ministry of Environment in 2019. The algorithm comprises three steps: preprocesses, radiance fitting, and postprocesses. The preprocesses include a wavelength calibration, as well as interpolation and convolution of absorption cross sections; radiance fitting is conducted using a nonlinear fitting method referred to as basic optical absorption spectroscopy (BOAS); and postprocesses include air mass factor calculations and bias corrections. In this study, several sensitivity tests are conducted to examine the retrieval uncertainties using the GEMS HCHO algorithm. We evaluate the algorithm with the Ozone Monitoring Instrument (OMI) Level 1B irradiance/radiance data by comparing our retrieved HCHO column densities with OMI HCHO products of the Smithsonian Astrophysical Observatory (OMHCHO) and of the Quality Assurance for Essential Climate Variables project (OMI QA4ECV). Results show that OMI HCHO slant columns retrieved using the GEMS algorithm are in good agreement with OMHCHO, with correlation coefficients of 0.77–0.91 and regression slopes of 0.94–1.04 for March, June, September, and December 2005. Spatial distributions of HCHO slant columns from the GEMS algorithm are consistent with the OMI QA4ECV products, but relatively poorer correlation coefficients of 0.52–0.76 are found compared to those against the OMHCHO products. Also, we compare the satellite results with ground-based multi-axis differential optical absorption spectroscopy (MAX-DOAS) observations. OMI GEMS HCHO vertical columns are 9 %–25 % lower than those of MAX-DOAS at Haute-Provence Observatory (OHP) in France, Bremen in Germany, and Xianghe in China. We find that the OMI GEMS retrievals have less bias than the OMHCHO and OMI QA4ECV products at OHP and Bremen in comparison with MAX-DOAS.

Ground-based MAX-DOAS observations of tropospheric formaldehyde VCDs and comparisons with the CAMS model at a rural site near Beijing during APEC 2014

Abstract. Formaldehyde (HCHO), a key aerosol precursor, plays a significant role in atmospheric photo-oxidation pathways. In this study, HCHO column densities were measured using a Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) instrument at the University of Chinese Academy of Science (UCAS) in Huairou District, Beijing, which is about 50 km away from the city center. Measurements were taken during the period of 1 October 2014 to 31 December 2014, and the Asia-Pacific Economic Cooperation (APEC) summit was organized on 5–11 November. Peak values of HCHO vertical column densities (VCDs) around noon and a good correlation coefficient R2 of 0.73 between HCHO VCDs and surface O3 concentration during noontime indicated that the secondary sources of HCHO through photochemical reactions of volatile organic compounds (VOCs) dominated the HCHO values in the area around UCAS. Dependences of HCHO VCDs on wind fields and backward trajectories were identified and indicated that the HCHO values in the area around UCAS were considerably affected by the transport of pollutants (VOCs) from polluted areas in the south. The effects of control measures on HCHO VCDs during the APEC period were evaluated. During the period of the APEC conference, the average HCHO VCDs were ∼38%±20% and ∼30%±24% lower than that during the pre-APEC and post-APEC periods calculated at the 95 % confidence limit, respectively. This phenomenon could be attributed to both the effects of prevailing northwest wind fields during APEC and strict control measures. We also compared the MAX-DOAS results with the Copernicus Atmosphere Monitoring Service (CAMS) model. The HCHO VCDs of the CAMS model and MAX-DOAS were generally consistent with a correlation coefficient R2 greater than 0.68. The peak values were consistently captured by both data datasets, but the low values were systematically underestimated by the CAMS model. This finding may indicate that the CAMS model can adequately simulate the effects of the transport and the secondary sources of HCHO but underestimates the local primary sources.