Abstract. Global observations of tropospheric nitrogen dioxide (NO2) columns have been shown to be feasible from space, but consistent multi-sensor records do not yet exist, nor are they covered by planned activities at the international level. Harmonised, multi-decadal records of NO2 columns and their associated uncertainties can provide crucial information on how the emissions and concentrations of nitrogen oxides evolve over time. Here we describe the development of a new, community best-practice NO2 retrieval algorithm based on a synthesis of existing approaches. Detailed comparisons of these approaches led us to implement an enhanced spectral fitting method for NO2, a 1° × 1° TM5-MP data assimilation scheme to estimate the stratospheric background and improve air mass factor calculations. Guided by the needs expressed by data users, producers, and WMO GCOS guidelines, we incorporated detailed per-pixel uncertainty information in the data product, along with easily traceable information on the relevant quality aspects of the retrieval. We applied the improved QA4ECV NO2 algorithm to the most current level-1 data sets to produce a complete 22-year data record that includes GOME (1995–2003), SCIAMACHY (2002–2012), GOME-2(A) (2007 onwards) and OMI (2004 onwards). The QA4ECV NO2 spectral fitting recommendations and TM5-MP stratospheric column and air mass factor approach are currently also applied to S5P-TROPOMI. The uncertainties in the QA4ECV tropospheric NO2 columns amount to typically 40 % over polluted scenes. The first validation results of the QA4ECV OMI NO2 columns and their uncertainties over Tai'an, China, in June 2006 suggest a small bias (−2 %) and better precision than suggested by uncertainty propagation. We conclude that our improved QA4ECV NO2 long-term data record is providing valuable information to quantitatively constrain emissions, deposition, and trends in nitrogen oxides on a global scale.
Abstract. We describe the new version 3.0 NASA Ozone Monitoring Instrument (OMI) standard nitrogen dioxide (NO 2 ) products (SPv3). The products and documentation are publicly available from the NASA Goddard Earth Sciences Data and Information Services Center (https://disc. gsfc.nasa.gov/datasets/OMNO2_V003/summary/). The major improvements include (1) a new spectral fitting algorithm for NO 2 slant column density (SCD) retrieval and (2) higherresolution (1 • latitude and 1.25 • longitude) a priori NO 2 and temperature profiles from the Global Modeling Initiative (GMI) chemistry-transport model with yearly varying emissions to calculate air mass factors (AMFs) required to convert SCDs into vertical column densities (VCDs). The new SCDs are systematically lower (by ∼ 10-40 %) than previous, version 2, estimates. Most of this reduction in SCDs is propagated into stratospheric VCDs. Tropospheric NO 2 VCDs are also reduced over polluted areas, especially over western Europe, the eastern US, and eastern China. Initial evaluation over unpolluted areas shows that the new SPv3 products agree better with independent satellite-and ground-based Fourier transform infrared (FTIR) measurements. However, further evaluation of tropospheric VCDs is needed over polluted areas, where the increased spatial resolution and more refined AMF estimates may lead to better characterization of pollution hot spots.
Abstract. The Tropospheric Monitoring Instrument (TROPOMI), aboard the Sentinel-5 Precursor (S5P) satellite, launched on 13 October 2017, provides measurements of atmospheric trace gases and of cloud and aerosol properties at an unprecedented spatial resolution of approximately 7×3.5 km2 (approx. 5.5×3.5 km2 as of 6 August 2019), achieving near-global coverage in 1 d. The retrieval of nitrogen dioxide (NO2) concentrations is a three-step procedure: slant column density (SCD) retrieval, separation of the SCD in its stratospheric and tropospheric components, and conversion of these into vertical column densities. This study focusses on the TROPOMI NO2 SCD retrieval: the retrieval method used, the stability of the SCDs and the SCD uncertainties, and a comparison with the Ozone Monitoring Instrument (OMI) NO2 SCDs. The statistical uncertainty, based on the spatial variability of the SCDs over a remote Pacific Ocean sector, is 8.63 µmol m−2 for all pixels (9.45 µmol m−2 for clear-sky pixels), which is very stable over time and some 30 % less than the long-term average over OMI–QA4ECV data (since the pixel size reduction TROPOMI uncertainties are ∼8 % larger). The SCD uncertainty reported by the differential optical absorption spectroscopy (DOAS) fit is about 10 % larger than the statistical uncertainty, while for OMI–QA4ECV the DOAS uncertainty is some 20 % larger than its statistical uncertainty. Comparison of the SCDs themselves over the Pacific Ocean, averaged over 1 month, shows that TROPOMI is about 5 % higher than OMI–QA4ECV, which seems to be due mainly to the use of the so-called intensity offset correction in OMI–QA4ECV but not in TROPOMI: turning that correction off means about 5 % higher SCDs. The row-to-row variation in the SCDs of TROPOMI, the “stripe amplitude”, is 2.15 µmol m−2, while for OMI–QA4ECV it is a factor of ∼2 (∼5) larger in 2005 (2018); still, a so-called stripe correction of this non-physical across-track variation is useful for TROPOMI data. In short, TROPOMI shows a superior performance compared with OMI–QA4ECV and operates as anticipated from instrument specifications. The TROPOMI data used in this study cover 30 April 2018 up to 31 January 2020.
Abstract. Nitrogen dioxide (NO2) and formaldehyde (HCHO) column data from satellite instruments are used for air quality and climate studies. Both NO2 and HCHO have been identified as precursors to the ozone (O3) and aerosol essential climate variables, and it is essential to quantify and characterise their uncertainties. Here we present an intercomparison of NO2 and HCHO slant column density (SCD) retrievals from four different research groups (BIRA-IASB, IUP Bremen, and KNMI as part of the Quality Assurance for Essential Climate Variables (QA4ECV) project consortium, and NASA) and from the OMI and GOME-2A instruments. Our evaluation is motivated by recent improvements in differential optical absorption spectroscopy (DOAS) fitting techniques and by the desire to provide a fully traceable uncertainty budget for the climate data record generated within QA4ECV. The improved NO2 and HCHO SCD values are in close agreement but with substantial differences in the reported uncertainties between groups and instruments. To check the DOAS uncertainties, we use an independent estimate based on the spatial variability of the SCDs within a remote region. For NO2, we find the smallest uncertainties from the new QA4ECV retrieval (0.8 × 1015 molec. cm−2 for both instruments over their mission lifetimes). Relative to earlier approaches, the QA4ECV NO2 retrieval shows better agreement between DOAS and statistical uncertainty estimates, suggesting that the improved QA4ECV NO2 retrieval has reduced but not altogether eliminated systematic errors in the fitting approach. For HCHO, we reach similar conclusions (QA4ECV uncertainties of 8–12 × 1015 molec. cm−2), but the closeness between the DOAS and statistical uncertainty estimates suggests that HCHO uncertainties are indeed dominated by random noise from the satellite's level 1 data. We find that SCD uncertainties are smallest for high top-of-atmosphere reflectance levels with high measurement signal-to-noise ratios. From 2005 to 2015, OMI NO2 SCD uncertainties increase by 1–2 % year−1, which is related to detector degradation and stripes, but OMI HCHO SCD uncertainties are remarkably stable (increase < 1 % year−1) and this is related to the use of Earth radiance reference spectra which reduces stripes. For GOME-2A, NO2 and HCHO SCD uncertainties increased by 7–9 and 11–15 % year−1 respectively up until September 2009, when heating of the instrument markedly reduced further throughput loss, stabilising the degradation of SCD uncertainty to < 3 % year−1 for 2009–2015. Our work suggests that the NO2 SCD uncertainty largely consists of a random component ( ∼ 65 % of the total uncertainty) as a result of the propagation of measurement noise but also of a substantial systematic component ( ∼ 35 % of the total uncertainty) mainly from stripe effects. Averaging over multiple pixels in space and/or time can significantly reduce the SCD uncertainties. This suggests that trend detection in OMI, GOME-2 NO2, and HCHO time series is not limited by the spectral fitting but rather by the adequacy of assumptions on the atmospheric state in the later air mass factor (AMF) calculation step.
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