The formaldehyde budget as seen by a global-scale multi-constraint and multi-species inversion system

Fortems-Cheiney, Audrey; Chevallier, F.; Pison, Isabelle; Bousquet, P.; Saunois, Marielle; Szopa, Sophie; Cressot, C.; Kurosu, Thomas P.; Chance, K.; Fried, Alan

doi:10.5194/acp-12-6699-2012

Cited by 106 publications

(104 citation statements)

References 76 publications

(96 reference statements)

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“…The formaldehyde seasonal variations are primarily related to the increase of biogenic emissions during local summer months at mid-latitudes over deciduous forests (in America, in Europe, in Northern Asia and in Australia), and during the dry season over evergreen tropical forests (in Amazon and Africa). In the Tropics, biomass burning also contributes significantly to the H 2 CO columns (Gonzi et al, 2011;Stavrakou et al, 2009b). Over the Amazon, burning is more widespread between September and November (SON) , while over Africa, a dipole pattern exists owing to different seasonal burning either side of the Equator (Stavrakou et al, 2009a;Marais et al, 2012).…”

Section: Error Analysis and Data Product Characterisationmentioning

confidence: 99%

“…Another important error source of the AMF calculation is the lack of correction in the case of absorbing aerosols, principally in biomass burning conditions. Indeed, it has been shown in several studies that the impact of aerosols on air mass factors is mainly significant when the aerosol layer is above the bulk of formaldehyde, and when the aerosol optical thickness is high, typical of biomass burning conditions (Leitão et al, 2010;Gonzi et al, 2011;Barkley et al, 2012). A full treatment of clouds and aerosols in radiative transfer will only be possible if clouds are aerosols are represented separately as scattering layers and if detailed information on aerosol optical properties is available at the global scale (Valks et al, 2011).…”

Section: Error Analysis and Data Product Characterisationmentioning

confidence: 99%

“…Palmer et al, 2006;Fu et al, 2007;Millet et al, 2008;Stavrakou et al, 2009b, c;Curci et al, 2010;Barkley et al, 2011;Fortems-Cheiney et al, 2012;Marais et al, 2012).…”

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confidence: 99%

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Improved retrieval of global tropospheric formaldehyde columns from GOME-2/MetOp-A addressing noise reduction and instrumental degradation issues

et al. 2012

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Abstract. We present a new dataset of formaldehyde vertical columns retrieved from observations of GOME-2 on board the EUMETSAT MetOp-A platform between 2007 and 2011. The new retrieval scheme, which has been optimised for GOME-2, includes a two-step fitting procedure that strongly reduces the impact of spectral interferences between H 2 CO and BrO, and a modified DOAS approach that better handles ozone absorption effects at moderately low sun elevations. Owing to these new features, the noise in the H 2 CO slant columns is reduced by up to 40 % in comparison to baseline retrieval settings used operationally. Also, the previously reported underestimation of the H 2 CO columns in tropical and mid-latitude regions has been largely eliminated, improving the agreement with coincident SCIAMACHY observations. To compensate for the drift of the GOME-2 slit function and to mitigate the instrumental degradation effects on H 2 CO retrievals, an asymmetric Gaussian line-shape is fitted during the irradiance calibration. Additionally, external parameters used in the tropospheric air mass factor computation (surface reflectances, cloud parameters and a priori profile shapes of H 2 CO) have been updated using most recent databases. Similar updates were also applied to the historical datasets of GOME and SCIAMACHY, leading to the generation of a consistent multi-mission H 2 CO data record covering the time period from 1997 until 2011. Comparing the resulting time series of monthly averaged H 2 CO vertical columns in 12 large regions worldwide, the correlation coefficient between SCIAMACHY and GOME-2 columns is generally higher than 0.8 in the overlap period, and linear regression slopes differ by less than 10 % from unity in most of the regions. In comparison to SCIAMACHY, the largely improved spatial sampling of GOME-2 allows for a better characterisation of formaldehyde distribution at the regional scale and/or at shorter timescales, leading to a better identification of the emission sources of non-methane volatile organic compounds.

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Section: Error Analysis and Data Product Characterisationmentioning

confidence: 99%

Section: Error Analysis and Data Product Characterisationmentioning

confidence: 99%

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Improved retrieval of global tropospheric formaldehyde columns from GOME-2/MetOp-A addressing noise reduction and instrumental degradation issues

et al. 2012

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“…Maximum HCHO concentrations can reach 100 ppb in polluted areas whereas sub-ppb levels are found in remote areas (Finlayson-Pitts and Pitts, 2000). Most of HCHO is produced during the oxidation of organic compounds (Fortems-Cheiney et al, 2012). While methane (CH 4 ) oxidation by OH radicals is the major source of HCHO in remote areas, the HCHO production in regions (e.g., forest, urban area) with elevated non-methane hydrocarbons (NMHCs) (i.e., alkanes, alkenes, aromatics, isoprene, and terpenes) is dominated by their degradation.…”

Section: Introductionmentioning

confidence: 99%

Modeling of HCHO and CHOCHO at a semi-rural site in southern China during the PRIDE-PRD2006 campaign

Rohrer²,

Brauers³

et al. 2014

Atmos. Chem. Phys.

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Abstract. HCHO and CHOCHO are important trace gases in the atmosphere, serving as tracers of VOC oxidations. In the past decade, high concentrations of HCHO and CHOCHO have been observed for the Pearl River Delta (PRD) region in southern China. In this study, we performed box model simulations of HCHO and CHOCHO at a semi-rural site in the PRD, focusing on understanding their sources and sinks and factors influencing the CHOCHO to HCHO ratio (R GF ). The model was constrained by the simultaneous measurements of trace gases and radicals. Isoprene oxidation by OH radicals is the major pathway forming HCHO, followed by degradations of alkenes, aromatics, and alkanes. The production of CHOCHO is dominated by isoprene and aromatic degradation; contributions from other NMHCs are of minor importance. Compared to the measurement results, the model predicts significant higher HCHO and CHOCHO concentrations. Sensitivity studies suggest that fresh emissions of precursor VOCs, uptake of HCHO and CHOCHO by aerosols, fast vertical transport, and uncertainties in the treatment of dry deposition all have the potential to contribute significantly to this discrepancy. Our study indicates that, in addition to chemical considerations (i.e., VOC composition, OH and NO x levels), atmospheric physical processes (e.g., transport, dilution, deposition) make it difficult to use the CHOCHO to HCHO ratio as an indicator for the origin of air mass composition.

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“…Tracing the observed HCHO back to the location of isoprene emission requires accounting for this coupling between chemistry and transport. Previous studies have 5 applied adjoint-based global inversions to account for transport in the isoprene-HCHO source-receptor relationship (Stavrakou et al, 2009;Fortems-Cheiney et al, 2012;Stavrakou et al, 2015;Bauwens et al, 2016), but they used older chemical mechanisms and horizontal resolutions of hundreds of km that do not capture the chemical time scales for isoprene conversion to HCHO.…”

mentioning

confidence: 99%

High-resolution inversion of OMI formaldehyde columns to quantify isoprene emission on ecosystem-relevant scales: application to the Southeast US

Kaiser¹,

Jacob²,

Zhu³

et al. 2017

Preprint

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Abstract. Isoprene emissions from vegetation have a large effect on atmospheric chemistry and air quality. isoprene emission inventories used in atmospheric models are based on limited vegetation information and uncertain land cover data, leading to potentially large errors. Satellite observations of atmospheric formaldehyde (HCHO), a high-yield isoprene oxidation product, provide 'top-down' information to evaluate isoprene emission inventories through inverse analyses. Past inverse analyses have however been hampered by uncertainty in the HCHO satellite data, uncertainty in the time-and NO x -dependent yield of HCHO from isoprene oxidation, and coarse resolution of the atmospheric models used for 30 the inversion. Here we demonstrate the ability to use HCHO satellite data from OMI in a high-resolution inversion to 2 to correct model NO x biases, which was done here using SEAC 4 RS observations but can be done more generally using satellite NO 2 data concurrently with HCHO. We find in our inversion that isoprene emissions from the widely-used MEGAN v2.1 inventory are biased high over the Southeast US by 40% on average, although the broad-scale distributions are correct including maximum emissions in Arkansas/Louisiana and high base emission factors in the oak-covered Ozarks of Southeast Missouri. A particularly large discrepancy is in the Edwards Plateau of Central Texas where MEGAN v2.1 is too high by a 5 factor of 3, possibly reflecting errors in land cover. The lower isoprene emissions inferred from our inversion, when implemented into GEOS-Chem, decrease surface ozone over the Southeast US by 1-3 ppb and decrease the isoprene contribution to organic aerosol from 40% to 20%.

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The formaldehyde budget as seen by a global-scale multi-constraint and multi-species inversion system

Cited by 106 publications

References 76 publications

Improved retrieval of global tropospheric formaldehyde columns from GOME-2/MetOp-A addressing noise reduction and instrumental degradation issues

Improved retrieval of global tropospheric formaldehyde columns from GOME-2/MetOp-A addressing noise reduction and instrumental degradation issues

Modeling of HCHO and CHOCHO at a semi-rural site in southern China during the PRIDE-PRD2006 campaign

High-resolution inversion of OMI formaldehyde columns to quantify isoprene emission on ecosystem-relevant scales: application to the Southeast US

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