scholarly journals Development and characterisation of a state-of-the-art GOME-2 formaldehyde air-mass factor algorithm

2015 ◽  
Vol 8 (1) ◽  
pp. 1109-1150 ◽  
Author(s):  
W. Hewson ◽  
M. P. Barkley ◽  
G. Gonzalez Abad ◽  
H. Bösch ◽  
T. Kurosu ◽  
...  

Abstract. Space-borne observations of formaldehyde (HCHO) are frequently used to derive surface emissions of isoprene, an important biogenic volatile organic compound. The conversion of retrieved HCHO slant column concentrations from satellite line of sight measurements to vertical columns is determined through application of an air mass factor (AMF), accounting for instrument viewing geometry, radiative transfer, and vertical profile of the absorber in the atmosphere. This step in the trace gas retrieval is subject to large errors. This work presents the AMF algorithm in use at the University of Leicester (UoL), which introduces scene specific variables into a per-observation full radiative transfer AMF calculation, including increasing spatial resolution of key environmental parameter databases, input variable area weighting, instrument specific scattering weight calculation, and inclusion of an ozone vertical profile climatology. Application of these updates to HCHO slant columns from the GOME-2 instrument is shown to typically adjust the AMF by ±10%, compared to a~reference algorithm without these advanced parameterisations. Furthermore, the new UoL algorithm also incorporates a full radiative transfer error calculation for each scene to help characterise AMF uncertainties. Global median AMF errors are typically 50–60%, and are dominated by uncertainties in the HCHO profile shape and its corresponding seasonal variation.

2015 ◽  
Vol 8 (10) ◽  
pp. 4055-4074 ◽  
Author(s):  
W. Hewson ◽  
M. P. Barkley ◽  
G. Gonzalez Abad ◽  
H. Bösch ◽  
T. Kurosu ◽  
...  

Abstract. Space-borne observations of formaldehyde (HCHO) are frequently used to derive surface emissions of isoprene, an important biogenic volatile organic compound. The conversion of retrieved HCHO slant column concentrations from satellite line-of-sight measurements to vertical columns is determined through application of an air mass factor (AMF), accounting for instrument viewing geometry, radiative transfer, and vertical profile of the absorber in the atmosphere. This step in the trace gas retrieval is subject to large errors. This work presents the AMF algorithm in use at the University of Leicester (UoL), which introduces scene-specific variables into a per-observation full radiative transfer AMF calculation, including increasing spatial resolution of key environmental parameter databases, input variable area weighting, instrument-specific scattering weight calculation, and inclusion of an ozone vertical profile climatology. Application of these updates to HCHO slant columns from the GOME-2 instrument is shown to typically adjust the AMF by ±20 %, compared to a reference algorithm without these advanced parameterisations. On average the GOME-2 AMFs increase by 4 %, with over 70 % of locations having an AMF of 0–20 % larger than originally, largely resulting from the use of the latest GOME-2 reflectance product. Furthermore, the new UoL algorithm also incorporates a full radiative transfer error calculation for each scene to help characterise AMF uncertainties. Global median AMF errors are typically 50–60 %, and are driven by uncertainties in the HCHO profile shape and its vertical distribution relative to clouds and aerosols. If uncertainty on the a priori HCHO profile is relatively small (< 10 %) then the median AMF total error decreases to about 30–40 %.


2017 ◽  
Vol 10 (3) ◽  
pp. 759-782 ◽  
Author(s):  
Alba Lorente ◽  
K. Folkert Boersma ◽  
Huan Yu ◽  
Steffen Dörner ◽  
Andreas Hilboll ◽  
...  

Abstract. Air mass factor (AMF) calculation is the largest source of uncertainty in NO2 and HCHO satellite retrievals in situations with enhanced trace gas concentrations in the lower troposphere. Structural uncertainty arises when different retrieval methodologies are applied within the scientific community to the same satellite observations. Here, we address the issue of AMF structural uncertainty via a detailed comparison of AMF calculation methods that are structurally different between seven retrieval groups for measurements from the Ozone Monitoring Instrument (OMI). We estimate the escalation of structural uncertainty in every sub-step of the AMF calculation process. This goes beyond the algorithm uncertainty estimates provided in state-of-the-art retrievals, which address the theoretical propagation of uncertainties for one particular retrieval algorithm only. We find that top-of-atmosphere reflectances simulated by four radiative transfer models (RTMs) (DAK, McArtim, SCIATRAN and VLIDORT) agree within 1.5 %. We find that different retrieval groups agree well in the calculations of altitude resolved AMFs from different RTMs (to within 3 %), and in the tropospheric AMFs (to within 6 %) as long as identical ancillary data (surface albedo, terrain height, cloud parameters and trace gas profile) and cloud and aerosol correction procedures are being used. Structural uncertainty increases sharply when retrieval groups use their preference for ancillary data, cloud and aerosol correction. On average, we estimate the AMF structural uncertainty to be 42 % over polluted regions and 31 % over unpolluted regions, mostly driven by substantial differences in the a priori trace gas profiles, surface albedo and cloud parameters. Sensitivity studies for one particular algorithm indicate that different cloud correction approaches result in substantial AMF differences in polluted conditions (5 to 40 % depending on cloud fraction and cloud pressure, and 11 % on average) even for low cloud fractions (<  0.2) and the choice of aerosol correction introduces an average uncertainty of 50 % for situations with high pollution and high aerosol loading. Our work shows that structural uncertainty in AMF calculations is significant and that it is mainly caused by the assumptions and choices made to represent the state of the atmosphere. In order to decide which approach and which ancillary data are best for AMF calculations, we call for well-designed validation exercises focusing on polluted conditions in which AMF structural uncertainty has the highest impact on NO2 and HCHO retrievals.


2016 ◽  
Author(s):  
Alba Lorente ◽  
K. Folkert Boersma ◽  
Huan Yu ◽  
Steffen Dörner ◽  
Andreas Hilboll ◽  
...  

Abstract. Air mass factor (AMF) calculation is the largest source of uncertainty in NO2 and HCHO satellite retrievals in situations with enhanced trace gas concentrations in the lower troposphere. Structural uncertainty arises when different retrieval methodologies are applied in the scientific community to the same satellite observations. Here, we address the issue of AMF structural uncertainty via a detailed comparison of AMF calculation methods that are structurally different between seven retrieval groups for measurements from the Ozone Monitoring Instrument (OMI). We estimate the escalation of structural uncertainty in every sub-step of the AMF calculation process. This goes beyond the algorithm uncertainty estimates provided in state-of-the-art retrievals, which address the theoretical propagation of uncertainties for one particular retrieval algorithm only. We find that top-of-atmosphere reflectances simulated by four radiative transfer models (RTMs) (DAK, McArtim, SCIATRAN and VLIDORT) agree within 1.5 %. We find that different retrieval groups agree well in the calculations of altitude resolved AMFs from different RTMs (to within 3 %), and in the tropospheric AMFs (to within 6 %) as long as identical ancillary data (surface albedo, terrain height, cloud parameters and trace gas profile) and cloud and aerosol correction procedures are being used. Structural uncertainty increases sharply when retrieval groups use their preference for ancillary data, cloud and aerosol correction. On average, we estimate the AMF structural uncertainty to be 42 % over polluted regions and 31 % over unpolluted regions, mostly driven by substantial differences in the a priori trace gas profiles, surface albedo and cloud parameters. Sensitivity studies for one particular algorithm indicate that different cloud correction approaches result in substantial AMF differences in polluted situations (5 to 40 % depending on cloud fraction and cloud pressure, and 11 % on average) even for low cloud fractions ( < 0.2) and the choice of aerosol correction introduces an average uncertainty of 50 % for situations with high pollution and high aerosol loading. Our work shows that structural uncertainty in AMF calculations is significant and that is mainly caused by the assumptions and choices made to represent the state of the atmosphere. To point out which approach and which ancillary data are the best for AMF calculations, we call for well-designed validation exercises focusing on polluted situations when AMF structural uncertainty has the highest impact on NO2 and HCHO retrievals.


2016 ◽  
Author(s):  
Lei Zhu ◽  
Daniel J. Jacob ◽  
Patrick S. Kim ◽  
Jenny A. Fisher ◽  
Karen Yu ◽  
...  

Abstract. Formaldehyde (HCHO) column data from satellites are widely used as a proxy for emissions of volatile organic compounds (VOCs), but validation of the data has been extremely limited. Here we use highly accurate HCHO aircraft observations from the NASA SEAC4RS campaign over the Southeast US in August–September 2013 to validate and intercompare six operational and research retrievals of HCHO columns from four different satellite instruments (OMI, GOME2A, GOME2B and OMPS) and three different research groups. The GEOS-Chem chemical transport model provides a common intercomparison platform. We find that all retrievals capture the HCHO maximum over Arkansas and Louisiana, reflecting high emissions of biogenic isoprene, and are consistent in their spatial variability over the Southeast US (r = 0.4–0.8 on a 0.5° × 0.5° grid) as well as their day-to-day variability (r = 0.5–0.8). However, all satellite retrievals are biased low in the mean by 20–51 %, which would lead to corresponding bias in estimates of isoprene emissions from the satellite data. The smallest bias is for OMI-BIRA, which has the highest corrected slant columns and the lowest scattering weights in its air mass factor (AMF) calculation. Correcting the assumed HCHO vertical profiles (shape factors) used in the AMF calculation would further reduce the bias in the OMI-BIRA data. We conclude that current satellite HCHO data provide a reliable proxy for isoprene emission variability but with a low mean bias due both to the corrected slant columns and the scattering weights used in the retrievals.


2012 ◽  
Vol 113 (9) ◽  
pp. 721-738 ◽  
Author(s):  
Timothy D. Hay ◽  
Greg E. Bodeker ◽  
Karin Kreher ◽  
Robyn Schofield ◽  
J. Ben Liley ◽  
...  

2019 ◽  
Author(s):  
Lisa K. Behrens ◽  
Andreas Hilboll ◽  
Andreas Richter ◽  
Enno Peters ◽  
Leonardo M. A. Alvarado ◽  
...  

Abstract. Trace gas maps retrieved from satellite measurements show enhanced levels of the atmospheric volatile organic compounds formaldehyde (HCHO) and glyoxal (CHOCHO) over the Atlantic Ocean. To validate the spatial distribution of this continental outflow, ship-based measurements were taken during the project Continental Outflow of Pollutants towards the MArine tRoposphere (COPMAR). A Multi-AXis Differential Optical Absorption Spectrometer (MAX-DOAS) was operated on board the research vessel (RV) Maria S. Merian during the cruise MSM58/2. This cruise was conducted in October 2016 from Ponta Delgada (Azores) to Cape Town (South Africa), crossing between Cape Verde and the African continent. The instrument was continuously scanning the horizon looking towards the African continent. Enhanced levels of HCHO and CHOCHO were found in the area of expected outflow during this cruise. The observed spatial gradients of HCHO and CHOCHO along the cruise track agree with the spatial distributions from satellite measurements and MOZART-4 model simulations. The continental outflow from the African continent is observed in an elevated layer, higher than 1000 m, and probably originates from biogenic emissions or biomass burning according to FLEXPART emission sensitivities.


2005 ◽  
Vol 5 (1) ◽  
pp. 17-66 ◽  
Author(s):  
J. Meyer ◽  
A. Bracher ◽  
A. Rozanov ◽  
A. C. Schlesier ◽  
H. Bovensmann ◽  
...  

Abstract. This presentation concentrates on solar occultation measurements with the spaceborne spectrometer SCIAMACHY in the UV-Vis wavelength range. Solar occultation measurements provide unique information about the vertical distribution of atmospheric constituents. For retrieval of vertical trace gas concentration profiles, an algorithm has been developed based on the optimal estimation method. The forward model is capable to simulate the extinction signals of different species as they occur in atmospheric transmission spectra obtained from occultation measurements. Furthermore, correction algorithms have been implemented to address shortcomings of the tangent height pre-processing and inhomogeneities of measured solar spectra. First results of O3 and NO2 vertical profile retrievals have been validated with data from ozone sondes and satellite based occultation instruments. The validation shows very promising results for SCIAMACHY O3 and NO2 values between 15 to 35 km with errors in the order of 10% and 15%, respectively.


2017 ◽  
Author(s):  
Lisa K. Behrens ◽  
Andreas Hilboll ◽  
Andreas Richter ◽  
Enno Peters ◽  
Henk Eskes ◽  
...  

Abstract. In this study, we present a novel NO2 DOAS retrieval in the ultraviolet (UV) spectral range for satellite observations from the Global Ozone Monitoring Instrument 2 on board EUMETSAT’s MetOp-A (GOME-2A) satellite. We compare the results to those from an established NO2 retrieval in the visible (vis) spectral range from the same instrument and infer information about the NO2 vertical profile shape in the troposphere. As expected, radiative transfer calculations for satellite geometries show that the sensitivity close to the ground is higher in the vis than in the UV spectral range. Consequently, NO2 slant column densities (SCDs) in the vis are usually higher than in the UV, if the NO2 is close to the surface. Therefore, these differences in NO2 SCDs between the two spectral ranges contain information on the vertical distribution of NO2 in the troposphere. We combine these results with radiative transfer calculations and simulated NO2 fields from the TM5 chemistry transport model to evaluate the simulated NO2 vertical distribution. We investigate regions representative for both anthropogenic and biomass burning NO2 pollution. Anthropogenic air pollution is mostly located in the boundary layer close to the surface, which is reflected by the large differences between UV and vis SCDs of ~ 60 %. Biomass burning NO2 in contrast is often uplifted into elevated layers above the boundary layer. This is best seen in tropical Africa south of the equator, where the biomass burning NO2 is well observed in the UV, and the difference between the two spectral ranges is only ~ 36 %. In tropical Africa north of the equator, however, the biomass burning NO2 is located closer to the ground, reducing its visibility. While not enabling a full retrieval of the vertical NO2 profile shape in the troposphere, our results can help to constrain the vertical profile of NO2 in the lower troposphere and, when analyzed together with simulated NO2 fields, can help interpret the model output.


2011 ◽  
Vol 11 (15) ◽  
pp. 7875-7891 ◽  
Author(s):  
G. M. Wolfe ◽  
J. A. Thornton ◽  
M. McKay ◽  
A. H. Goldstein

Abstract. Understanding the fate of ozone within and above forested environments is vital to assessing the anthropogenic impact on ecosystems and air quality at the urban-rural interface. Observed forest-atmosphere exchange of ozone is often much faster than explicable by stomatal uptake alone, suggesting the presence of additional ozone sinks within the canopy. Using the Chemistry of Atmosphere-Forest Exchange (CAFE) model in conjunction with summer noontime observations from the 2007 Biosphere Effects on Aerosols and Photochemistry Experiment (BEARPEX-2007), we explore the viability and implications of the hypothesis that ozonolysis of very reactive but yet unidentified biogenic volatile organic compounds (BVOC) can influence the forest-atmosphere exchange of ozone. Non-stomatal processes typically generate 67 % of the observed ozone flux, but reactions of ozone with measured BVOC, including monoterpenes and sesquiterpenes, can account for only 2 % of this flux during the selected timeframe. By incorporating additional emissions and chemistry of a proxy for very reactive VOC (VRVOC) that undergo rapid ozonolysis, we demonstrate that an in-canopy chemical ozone sink of ~2 × 108 molec cm−3 s−1 can close the ozone flux budget. Even in such a case, the 65 min chemical lifetime of ozone is much longer than the canopy residence time of ~2 min, highlighting that chemistry can influence reactive trace gas exchange even when it is "slow" relative to vertical mixing. This level of VRVOC ozonolysis could enhance OH and RO2 production by as much as 1 pptv s−1 and substantially alter their respective vertical profiles depending on the actual product yields. Reaction products would also contribute significantly to the oxidized VOC budget and, by extension, secondary organic aerosol mass. Given the potentially significant ramifications of a chemical ozone flux for both in-canopy chemistry and estimates of ozone deposition, future efforts should focus on quantifying both ozone reactivity and non-stomatal (e.g. cuticular) deposition within the forest.


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