Abstract Ground‐based measurements of tropospheric ozone (O 3 ) are valuable for studies of atmospheric chemistry, air pollution, climate change, and for satellite validation. The Multi Axis Differential Optical Absorption Spectroscopy (MAX‐DOAS) technique has been widely used to derive vertical profiles of trace gases and aerosols in the troposphere. However, tropospheric O 3 has not yet been satisfactorily derived from MAX‐DOAS measurements due to the influence of stratospheric O 3 absorption. In this study, we developed two new retrieval approaches for tropospheric O 3 from MAX‐DOAS measurements. In method 1, stratospheric O 3 profiles from external data sources are considered in the retrieval. In method 2, stratospheric and tropospheric O 3 are separated based on the temperature‐dependent differences between tropospheric and stratospheric O 3 absorption structures in the UV spectral range. The feasibility of both methods is first verified by applying them to synthetic spectra. Then they are applied to real MAX‐DOAS measurements recorded during the CINDI‐2 campaign in Cabauw, the Netherlands (September 2016). The obtained results are compared with independent O 3 measurements and global chemical transport model simulations. Good agreement of the near‐surface O 3 concentrations with the independent data sets is found for both methods. However, tropospheric O 3 profiles are only reasonably derived using method 1, while they are significantly overestimated at altitudes above 1 km using method 2, probably due to the approximation of the ring spectra used to correct the rotational Raman scattering structures in the DOAS fit. Advantages and disadvantages of both methods are discussed and improvement directions are suggested for further studies.
Abstract. We present a new product with explicit aerosol corrections, POMINO-TROPOMI, for tropospheric nitrogen dioxide (NO2) vertical column densities (VCDs) over East Asia, based on the newly launched TROPOspheric Monitoring Instrument with an unprecedented high horizontal resolution. Compared to the official TM5-MP-DOMINO (OFFLINE) product, POMINO-TROPOMI shows stronger concentration gradients near emission source locations and better agrees with MAX-DOAS measurements (R2 = 0.75, NMB = 0.8 % versus R2 = 0.68, NMB = 41.9 %). Sensitivity tests suggest that implicit aerosol corrections, as in TM5-MP-DOMINO, lead to underestimations of NO2 columns by about 25 % over the polluted Northern East China region. Reducing the horizontal resolution of a priori NO2 profiles would underestimate the retrieved NO2 columns over isolated city clusters in western China by 35 % but with overestimates by more than 50 % over many offshore coastal areas. The effect of a priori NO2 profiles is more important under calm conditions.
Abstract. The COVID-19 lockdown had a large impact on anthropogenic emissions of air pollutants and particularly on nitrogen dioxide (NO2). While the overall NO2 decline over some large cities is well-established, understanding the details remains a challenge since multiple source categories contribute. In this study, a new method of isolation of three components (background NO2, NO2 from urban sources, and NO2 from industrial point sources) is applied to estimate the impact of the COVID-19 lockdown on each of them. The approach is based on fitting satellite data by a statistical model with empirical plume dispersion functions driven by a meteorological reanalysis. Population density and surface elevation data as well as coordinates of industrial sources were used in the analysis. The tropospheric NO2 vertical column density (VCD) values measured by the Tropospheric Monitoring Instrument (TROPOMI) on board the Sentinel-5 Precursor over 261 urban areas for the period from 16 March to 15 June 2020 were compared with the average VCD values for the same period in 2018 and 2019. While the background NO2 component remained almost unchanged, the urban NO2 component declined by −18 % to −28 % over most regions. India, South America, and a part of Europe (particularly, Italy, France, and Spain) demonstrated a −40 % to −50 % urban emission decline. In contrast, the decline over urban areas in China, where the lockdown was over during the analysed period, was, on average, only -4.4±8 %. Emissions from large industrial sources in the analysed urban areas varied greatly from region to region from -4.8±6 % for China to -40±10 % for India. Estimated changes in urban emissions are correlated with changes in Google mobility data (the correlation coefficient is 0.62) confirming that changes in traffic were one of the key elements in the decline in urban NO2 emissions. No correlation was found between changes in background NO2 and Google mobility data. On the global scale, the background and urban components were remarkably stable in 2018, 2019, and 2021, with averages of all analysed areas all being within ±2.5 % and suggesting that there were no substantial drifts or shifts in TROPOMI data. The 2020 data are clearly an outlier: in 2020, the mean background component for all analysed areas (without China) was -6.0%±1.2 % and the mean urban component was -26.7±2.6 % or 20σ below the baseline level from the other years.
In this work, we investigate the ability of a data assimilation technique and space-borne observations to quantify and monitor changes in nitrogen oxides (NOx) emissions over Northwestern Greece for the summers of 2018 and 2019. In this region, four lignite-burning power plants are located. The data assimilation technique, based on the Ensemble Kalman Filter method, is employed to combine space-borne atmospheric observations from the high spatial resolution Sentinel-5 Precursor (S5P) Tropospheric Monitoring Instrument (TROPOMI) and simulations using the LOTOS-EUROS Chemical Transport model. The Copernicus Atmosphere Monitoring Service-Regional European emissions (CAMS-REG, version 4.2) inventory based on the year 2015 is used as the a priori emissions in the simulations. Surface measurements of nitrogen dioxide (NO2) from air quality stations operating in the region are compared with the model surface NO2 output using either the a priori (base run) or the a posteriori (assimilated run) NOx emissions. Relative to the a priori emissions, the assimilation suggests a strong decrease in concentrations for the station located near the largest power plant, by 80% in 2019 and by 67% in 2018. Concerning the estimated annual a posteriori NOx emissions, it was found that, for the pixels hosting the two largest power plants, the assimilated run results in emissions decreased by ~40–50% for 2018 compared to 2015, whereas a larger decrease, of ~70% for both power plants, was found for 2019, after assimilating the space-born observations. For the same power plants, the European Pollutant Release and Transfer Register (E-PRTR) reports decreased emissions in 2018 and 2019 compared to 2015 (−35% and −38% in 2018, −62% and −72% in 2019), in good agreement with the estimated emissions. We further compare the a posteriori emissions to the reported energy production of the power plants during the summer of 2018 and 2019. Mean decreases of about −35% and−63% in NOx emissions are estimated for the two larger power plants in summer of 2018 and 2019, respectively, which are supported by similar decreases in the reported energy production of the power plants (~−30% and −70%, respectively).
Abstract. We present a new algorithm for the near-real time retrieval – within 3 h of the actual satellite measurement – of tropospheric NO2 columns from the Ozone Monitoring Instrument (OMI). The retrieval is based on the combined retrieval-assimilation-modelling approach developed at KNMI for off-line tropospheric NO2 from the GOME and SCIAMACHY satellite instruments. We have adapted the off-line system such that the required a priori information – profile shapes and stratospheric background NO2 – is now immediately available upon arrival (within 80 min of observation) of the OMI NO2 slant columns and cloud data at KNMI. Slant columns for NO2 are retrieved using differential optical absorption spectroscopy (DOAS) in the 405–465 nm range. Cloud fraction and cloud pressure are provided by a new cloud retrieval algorithm that uses the absorption of the O2-O2 collision complex near 477 nm. On-line availability of stratospheric slant columns and NO2 profiles is achieved by running the TM4 chemistry transport model (CTM) forward in time based on forecast ECMWF meteo and assimilated NO2 information from all previously observed orbits. OMI NO2 slant columns, after correction for spurious across-track variability, show a random error for individual pixels of approximately 0.7×1015 molec cm−2. Cloud parameters from OMI's O2-O2 algorithm have similar frequency distributions as retrieved from SCIAMACHY's Fast Retrieval Scheme for Cloud Observables (FRESCO) for August 2006. On average, OMI cloud fractions are higher by 0.011, and OMI cloud pressures exceed FRESCO cloud pressures by 60 hPa. A sequence of OMI observations over Europe in October 2005 shows OMI's capability to track changeable NOx air pollution from day to day in cloud-free situations.
The aim of this paper is to evaluate the surface concentration of nitrogen dioxide (NO2) inferred from the Sentinel-5 Precursor Tropospheric Monitoring Instrument (S5P/TROPOMI) NO2 tropospheric column densities over Central Europe for two time periods, summer 2019 and winter 2019–2020. Simulations of the NO2 tropospheric vertical column densities and surface concentrations from the Long-Term Ozone Simulation–European Operational Smog (LOTOS-EUROS) chemical transport model are also applied in the methodology. More than two hundred in situ air quality monitoring stations, reporting to the European Environment Agency (EEA) air quality database, are used to carry out comparisons with the model simulations and the spaceborne inferred surface concentrations. Stations are separated into seven types (urban traffic, suburban traffic, urban background, suburban background, rural background, suburban industrial and rural industrial) in order to examine the strengths and shortcomings of the different air quality markers, namely the NO2 vertical column densities and NO2 surface concentrations. S5P/TROPOMI NO2 surface concentrations are inferred by multiplying the fraction of the satellite and model NO2 vertical column densities with the model surface concentrations. The estimated inferred TROPOMI NO2 surface concentrations are examined further with the altering of three influencing factors: the model vertical leveling scheme, the versions of the TROPOMI NO2 data and the air mass factors applied to the satellite and model NO2 vertical column densities. Overall, the inferred TROPOMI NO2 surface concentrations show a better correlation with the in situ measurements for both time periods and all station types, especially for the industrial stations (R > 0.6) in winter. The calculated correlation for background stations is moderate for both periods (R~0.5 in summer and R > 0.5 in winter), whereas for traffic stations it improves in the winter (from 0.20 to 0.50). After the implementation of the air mass factors from the local model, the bias is significantly reduced for most of the station types, especially in winter for the background stations, ranging from +0.49% for the urban background to +10.37% for the rural background stations. The mean relative bias in winter between the inferred S5P/TROPOMI NO2 surface concentrations and the ground-based measurements for industrial stations is about −15%, whereas for traffic urban stations it is approximately −25%. In summer, biases are generally higher for all station types, especially for the traffic stations (~−75%), ranging from −54% to −30% for the background and industrial stations.
Lightning produces NO because the extreme temperatures (>20000 K) in lightning channels dissociate molecular O2 and molecular N2, which then combine to form NOx which quickly reacts with O3 to form NO2. Lightning is responsible for 10-15% of NOx emissions globally. This is 2 – 8 Tg N a-1 [Schumann and Huntrieser, 2007] or 100 to 400 mol per flash. Much of the uncertainty stems from limited knowledge of lightning NOx production per flash (LNOx PE) or per unit flash length. Most LNOx is injected into mid- and upper-troposphere where away from deep convection its lifetime is longer relative to lower troposphere NOx. NOx in this region enhances the concentrations of upper tropospheric NOy, OH, and O3 and contributes to positive radiative forcing by O3 and negative forcing by CH4. We have previously used OMI NO2 to obtain estimates of LNOx production per flash over the Gulf of Mexico (Pickering et al., 2016, JGR), in convective events during NASA’s TC4 field program (Bucsela et al., 2010, JGR), and over broad regions of the tropics (Allen et al., 2019, JGR) and midlatitudes (Bucsela et al., 2019, JGR). In the latter studies, we obtained PE values of 170 ± 100 mol flash and 180 ± 100 mol flash, respectively.
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