Spaceborne NO2 column observations from two high‐resolution instruments, Tropospheric Monitoring Instrument (TROPOMI) on board Sentinel‐5 Precursor and Ozone Monitoring Instrument (OMI) on Aura, reveal unprecedented NO2 decreases over China, South Korea, western Europe, and the United States as a result of public health measures enforced to contain the coronavirus disease outbreak (Covid‐19) in January–April 2020. The average NO2 column drop over all Chinese cities amounts to −40% relative to the same period in 2019 and reaches up to a factor of ~2 at heavily hit cities, for example, Wuhan, Jinan, while the decreases in western Europe and the United States are also significant (−20% to −38%). In contrast with this, although Iran is also strongly affected by the disease, the observations do not show evidence of lower emissions, reflecting more limited health measures.

Abstract. Due to the scarcity of observational constraints and the rapidly changing environment in East and Southeast Asia, isoprene emissions predicted by models are expected to bear substantial uncertainties. The aim of this study is to improve upon the existing bottom-up estimates, and to investigate the temporal evolution of the fluxes in Asia over 1979-2012. To this purpose, we calculate the hourly emissions at 0.5 • × 0.5 • resolution using the MEGAN-MOHYCAN model driven by ECMWF ERA-Interim climatology. In order to remedy for known biases identified in previous studies, and to improve the simulation of interannual variability and trends in emissions, this study incorporates (i) changes in land use, including the rapid expansion of oil palms, (ii) meteorological variability according to ERA-Interim, (iii) long-term changes in solar radiation (dimming/brightening) constrained by surface network radiation measurements, and (iv) recent experimental evidence that South Asian tropical forests are much weaker isoprene emitters than previously assumed, and on the other hand, that oil palms have a strong isoprene emission capacity. These effects lead to a significant lowering (factor of 2) in the total isoprene fluxes over the studied domain, and to emission reductions reaching a factor of 3.5 in Southeast Asia. The bottom-up annual isoprene emissions for 2005 are estimated at 7.0, 4.8, 8.3, and 2.9 Tg in China, India, Indonesia and Malaysia, respectively. The isoprene flux anomaly over the whole domain and studied period is found to be strongly correlated with the Oceanic Niño Index (r = 0.73), with positive (negative) anomalies related to El Niño (La Niña) years.Changes in temperature and solar radiation are the major drivers of the interannual variability and trends in the emissions, except over semi-arid areas such as northwestern China, Pakistan and Kazakhstan, where soil moisture is by far the main cause of interannual emission changes. In our base simulation, annual positive flux trends of 0.2 % and 0.52 % throughout the entire period are found in Asia and China, respectively, related to a positive trend in temperature and solar radiation. The impact of oil palm expansion in Indonesia and Malaysia is to enhance the trends over that region, e.g., from 1.17 % to 1.5 % in 1979-2005 in Malaysia. A negative emission trend is derived in India (−0.4 %), owing to the negative trend in solar radiation data associated with the strong dimming effect likely due to increasing aerosol loadings.The bottom-up emissions are compared to field campaign measurements in Borneo and South China and further evaluated against top-down isoprene emission estimates constrained by GOME-2/MetOp-A formaldehyde columns through 2007-2012. The satellite-based estimates appear to support our assumptions, and confirm the lower emission rate in tropical forests of Indonesia and Malaysia. Additional flux measurements are clearly needed to characterize the spatial variability of emission factors better. Finally, a decreasing trend in the inferr...

As formaldehyde (HCHO) is a high-yield product in the oxidation of most volatile organic compounds (VOCs) emitted by fires, vegetation, and anthropogenic activities, satellite observations of HCHO are well-suited to inform us on the spatial and temporal variability of the underlying VOC sources. The long record of space-based HCHO column observations from the Ozone Monitoring Instrument (OMI) is used to infer emission flux estimates from pyrogenic and biogenic volatile organic compounds (VOCs) on the global scale over 2005-2013. This is realized through the method of source inverse modeling, which consists in the optimization of emissions in a chemistry-transport model (CTM) in order to minimize the discrepancy between the observed and modeled HCHO columns. The top-down fluxes are derived in the global CTM IMAGESv2 by an iterative minimization algorithm based on the full adjoint of IMAGESv2, starting from a priori emission estimates provided by the newly released GFED4s (Global Fire Emission Database, version 4s) inventory for fires, and by the MEGAN-MOHYCAN inventory for isoprene emissions. The top-down fluxes are compared to two independent inventories for fire (GFAS and FINNv1.5) and isoprene emissions (MEGAN-MACC and GUESS-ES). The inversion indicates a moderate decrease (ca. 20 %) in the average annual global fire and isoprene emissions, from 2028 Tg C in the a priori to 1653 Tg C for burned biomass, and from 343 to 272 Tg for isoprene fluxes. Those estimates are acknowledged to depend on the accuracy of formaldehyde data, as well as on the assumed fire emission factors and the oxidation mechanisms leading to HCHO production. Strongly decreased top-down fire fluxes (30-50 %) are inferred in the peak fire season in Africa and during years with strong a priori fluxes associated with forest fires in Amazonia (in 2005, 2007, and 2010), bushfires in Australia (in 2006 and 2011), and peat burning in Indonesia (in 2006 and 2009), whereas generally increased fluxes are suggested in Indochina and during the 2007 fires in southern Europe. Moreover, changes in fire seasonal patterns are suggested; e.g., the seasonal amplitude is reduced over southeast Asia. In Africa, the inversion indicates increased fluxes due to agricultural fires and decreased maxima when natural fires are dominant. The top-down fire emissions are much better correlated with MODIS fire counts than the a priori inventory in regions with small and agricultural fires, indicating that the OMI-based inversion is well-suited to assess the associated emissions. Regarding biogenic sources, significant reductions in isoprene fluxes are inferred in tropical ecosystems (30-40 %), suggesting overestimated basal emission rates in those areas in the bottom-up inventory, whereas strongly positive isoprene emission updates are derived over semiarid and desert areas, especially in southern Africa and Australia. This finding suggests that the parameterization of the soil moisture stress used in MEGAN greatly exaggerates the flux reduction due to drought in those reg...

International audienceThe vertical columns of formaldehyde (HCHO) retrieved from two satellite instruments, the Global Ozone Monitoring Instrument-2 (GOME-2) on Metop-A and the Ozone Monitoring Instrument (OMI) on Aura, are used to constrain global emissions of HCHO precursors from open fires, vegetation and human activities in the year 2010. To this end, the emissions are varied and optimized using the adjoint model technique in the IMAGESv2 global CTM (chemistry-transport model) on a monthly basis and at the model resolution. Given the different local overpass times of GOME-2 (09:30 LT) and OMI (13:30 LT), the simulated diurnal cycle of HCHO columns is investigated and evaluated against ground-based optical measurements at 7 sites in Europe, China and Africa. The modelled diurnal cycle exhibits large variability, reflecting competition between photochemistry and emission variations, with noon or early afternoon maxima at remote locations (oceans) and in regions dominated by anthropogenic emissions, late afternoon or evening maxima over fire scenes, and midday minima in isoprene-rich regions. The agreement between simulated and ground-based columns is found to be generally better in summer (with a clear afternoon maximum at mid-latitude sites) than in winter, and the annually averaged ratio of afternoon to morning columns is slightly higher in the model (1.126) than in the ground-based measurements (1.043). The anthropogenic VOC (volatile organic compound) sources are found to be weakly constrained by the inversions on the global scale, mainly owing to their generally minor contribution to the HCHO columns, except over strongly polluted regions, like China. The OMI-based inversion yields total flux estimates over China close to the bottom-up inventory (24.6 vs. 25.5 in the a priori) with, however, pronounced increases in the Northeast China and reductions in the south. Lower fluxes are estimated based on GOME-2 HCHO columns (20.6 TgVOC), in particular over the Northeast, likely reflecting mismatches between the observed and the modelled diurnal cycle in this region. The resulting biogenic and pyrogenic flux estimates from both optimizations generally show a good degree of consistency. A reduction of the global annual biogenic emissions of isoprene is derived, by 9 and by 13% according to GOME-2 and OMI, respectively, compared to the a priori estimate of 363 Tg in 2010. The reduction is largest (up to 25–40%) in the Southeastern US, in accordance with earlier studies. The GOME-2 and OMI satellite columns suggest a global pyrogenic flux decrease by 36 and 33%, respectively, compared to the GFEDv3 inventory. This decrease is especially pronounced over tropical forests such as Amazonia and Thailand/Myanmar, and is supported by comparisons with IASI CO observations. In contrast to these flux reductions, the emissions due to harvest waste burning are strongly enhanced in the Northeastern China plain in June (by ca. 70% in June according to OMI) as well as over Indochina in March. Sensitivity inversions showed robustne...

The large-scale burning of crop residues in the North China Plain (NCP), one of the most densely populated world regions, was recently recognized to cause severe air pollution and harmful health effects. A reliable quantification of the magnitude of these fires is needed to assess regional air quality. Here, we use an eight-year record (2005–2012) of formaldehyde measurements from space to constrain the emissions of volatile organic compounds (VOCs) in this region. Using inverse modelling, we derive that satellite-based post-harvest burning fluxes are, on average, at least a factor of 2 higher than state-of-the-art bottom-up statistical estimates, although with significant interannual variability. Crop burning is calculated to cause important increases in surface ozone (+7%) and fine aerosol concentrations (+18%) in the North China Plain in June. The impact of crop fires is also found in satellite observations of other species, glyoxal, nitrogen dioxide and methanol, and we show that those measurements validate the magnitude of the top-down fluxes. Our study indicates that the top-down crop burning fluxes of VOCs in June exceed by almost a factor of 2 the combined emissions from other anthropogenic activities in this region, underscoring the need for targeted actions towards changes in agricultural management practices.

Abstract. Among the more than 20 ground-based FTIR (Fourier transform infrared) stations currently operating around the globe, only a few have provided formaldehyde (HCHO) total column time series until now. Although several independent studies have shown that the FTIR measurements can provide formaldehyde total columns with good precision, the spatial coverage has not been optimal for providing good diagnostics for satellite or model validation. Furthermore, these past studies used different retrieval settings, and biases as large as 50 % can be observed in the HCHO total columns depending on these retrieval choices, which is also a weakness for validation studies combining data from different ground-based stations.For the present work, the HCHO retrieval settings have been optimized based on experience gained from past studies and have been applied consistently at the 21 participating stations. Most of them are either part of the Network for the Detection of Atmospheric Composition Change (NDACC) or under consideration for membership. We provide the harmonized settings and a characterization of the HCHO FTIR products. Depending on the station, the total systematic and random uncertainties of an individual HCHO total column measurement lie between 12 % and 27 % and between 1 and 11×1014 molec cm−2, respectively. The median values among all stations are 13 % and 2.9×1014 molec cm−2 for the total systematic and random uncertainties.This unprecedented harmonized formaldehyde data set from 21 ground-based FTIR stations is presented and its comparison with a global chemistry transport model shows consistency in absolute values as well as in seasonal cycles. The network covers very different concentration levels of formaldehyde, from very clean levels at the limit of detection (few 1013 molec cm−2) to highly polluted levels (7×1016 molec cm−2). Because the measurements can be made at any time during daylight, the diurnal cycle can be observed and is found to be significant at many stations. These HCHO time series, some of them starting in the 1990s, are crucial for past and present satellite validation and will be extended in the coming years for the next generation of satellite missions.

As formaldehyde (HCHO) is a high-yield product in the oxidation of most volatile organic compounds (VOCs) emitted by fires, vegetation, and anthropogenic activities, satellite observations of HCHO are well-suited to inform us on the spatial and temporal variability of the underlying VOC sources. The long record of space-based HCHO column observations from the Ozone Monitoring Instrument (OMI) is used to infer emission flux estimates from pyrogenic and biogenic volatile organic compounds (VOCs) on the global scale over 2005-2013. This is realized through the method of source inverse modeling, which consists in the optimization of emissions in a chemistry-transport model (CTM) in order to minimize the discrepancy between the observed and modeled HCHO columns. The top-down fluxes are derived in the global CTM IMAGESv2 by an iterative minimization algorithm based on the full adjoint of IMAGESv2, starting from a priori emission estimates provided by the newly released GFED4s (Global Fire Emission Database, version 4s) inventory for fires, and by the MEGAN-MOHYCAN inventory for isoprene emissions. The top-down fluxes are compared to two independent inventories for fire (GFAS and FINNv1.5) and isoprene emissions (MEGAN-MACC and GUESS-ES). The inversion indicates a moderate decrease (ca. 20 %) in the average annual global fire and isoprene emissions, from 2028 Tg C in the a priori to 1653 Tg C for burned biomass, and from 343 to 272 Tg for isoprene fluxes. Those estimates are acknowledged to depend on the accuracy of formaldehyde data, as well as on the assumed fire emission factors and the oxidation mechanisms leading to HCHO production. Strongly decreased top-down fire fluxes (30-50 %) are inferred in the peak fire season in Africa and during years with strong a priori fluxes associated with forest fires in Amazonia (in 2005, 2007, and 2010), bushfires in Australia (in 2006 and 2011), and peat burning in Indonesia (in 2006 and 2009), whereas generally increased fluxes are suggested in Indochina and during the 2007 fires in southern Europe. Moreover, changes in fire seasonal patterns are suggested; e.g., the seasonal amplitude is reduced over southeast Asia. In Africa, the inversion indicates increased fluxes due to agricultural fires and decreased maxima when natural fires are dominant. The top-down fire emissions are much better correlated with MODIS fire counts than the a priori inventory in regions with small and agricultural fires, indicating that the OMI-based inversion is well-suited to assess the associated emissions. Regarding biogenic sources, significant reductions in isoprene fluxes are inferred in tropical ecosystems (30-40 %), suggesting overestimated basal emission rates in those areas in the bottom-up inventory, whereas strongly positive isoprene emission updates are derived over semiarid and desert areas, especially in southern Africa and Australia. This finding suggests that the parameterization of the soil moisture stress used in MEGAN greatly exaggerates the flux reduction due to drought in those reg...

Anthropogenic activities, by far the largest source of nox into the atmosphere, induce a weekly cycle of no 2 abundances in cities. Comprehensive analysis of the 2005-2017 OMI NO 2 dataset reveals significant weekly cycles in 115 of the 274 cities considered. These results are corroborated by a full year of highresolution tRopoMi no 2 observations. the oMi dataset permits us to identify trends in the weekly cycle resulting from nox emissions changes. the data show a clear weakening of the weekly cycle over european and U.S. cities, an evolution attributed to the decline in anthropogenic emissions and the resulting growing importance of background no 2 , whereas no 2 lifetime changes also play a minor role. in particular, the Sunday no 2 columns averaged over all U.S. cities are found to increase, relative to the weekly average, from 0.72 during 2005-2007 to 0.88 in 2015-2017. The opposite tendency is recorded in regions undergoing rapid emission growth. Multiyear simulations over the U.S. and the Middle east using the chemistry-transport model MAGRITTEv1.1 succeed in capturing the observed weekly cycles over the largest cities, as well as the observed long-term trends in the weekly cycle. Nitrogen oxides (NOx = NO 2 + NO) play a key role in atmospheric chemistry: they catalyse tropospheric ozone formation, they impact the self-cleaning capacity of the atmosphere, and they are precursors of secondary inorganic aerosol, with consequences for climate and human health 1. Fossil fuel combustion is the dominant source of NOx in the atmosphere, estimated at ~60% of the global total, whereas emissions from vegetation fires, lightning and soils make up the rest 2. Because of their relation to human activities, anthropogenic NOx emissions often display a weekly cycle, with reduced NOx levels in and around cities on rest days. Similar cycles have been also observed for other pollutants, e.g. aerosols 3,4 , and for meteorological parameters such as cloudiness 4,5. The NOx weekly cycle was previously investigated using ground-based, aircraft and satellite measurements 6-8 , whereas spatial patterns observed from satellites were used to study the urban photochemistry with the help of models 9. These studies, however, rely either on relatively short data records of at most several months 8,9 or on satellite data from coarse resolution sounders 6,7. Here we use NO 2 column data from two nadir-viewing satellite sensors, the Ozone Monitoring Instrument (OMI 10) launched in July 2004, and the high-resolution Tropospheric Monitoring Instrument (TROPOMI), single payload of the Sentinel-5 Precursor (S5P) launched in October 2017 11. Both sensors have an equatorial crossing time of ca. 13:40 (local time), and provide daily global coverage at resolutions of 13 × 24 km 2 and 7.2 × 3.5 km 2 (at nadir) for OMI and TROPOMI, respectively. The long data record compiled for this study (2005-2019) and the high resolution of both instruments allows to provide more robust information on the NO 2 weekly cycle over a larger number of cities around ...