Global upper-tropospheric formaldehyde: seasonal cycles observed by the ACE-FTS satellite instrument

Dufour, G.; Szopa, Sophie; Barkley, M. P.; Boone, C. D.; Perrin, A.; Palmer, Paul I.; Bernath, Peter F.

doi:10.5194/acp-9-3893-2009

Cited by 41 publications

(23 citation statements)

References 71 publications

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“…A similar latitudinal behaviour can be expected for HCHO, which was indeed found in the marine boundary layer (Arlander et al, 1995;Weller et al, 2000;Fried et al, 2002Fried et al, , 2003a but is less pronounced in the upper troposphere (Dufour et al, 2009).…”

Section: Introductionsupporting

confidence: 52%

Distribution of hydrogen peroxide and formaldehyde over Central Europe during the HOOVER project

et al. 2011

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Abstract. In this study we report measurements of hydrogen peroxide (H 2 O 2 ), methyl hydroperoxide* (MHP* as a proxy of MHP based on an unspecific measurement of total organic peroxides) and formaldehyde (HCHO) from the HO x OVer EuRope (HOOVER) project (HO x = OH+HO 2 ). HOOVER included two airborne field campaigns, in October 2006 and July 2007. Measurement flights were conducted from the base of operation Hohn (Germany, 54 • N, 9 • E) towards the Mediterranean and to the subpolar regions over Norway. We find negative concentration gradients with increasing latitude throughout the troposphere for H 2 O 2 and CH 3 OOH * . In contrast, observed HCHO is almost homogeneously distributed over central and northern Europe and is elevated over the Mediterranean. In general, the measured gradients tend to be steepest entering the Mediterranean region, where we also find the highest abundances of the 3 species. Mixing ratios of these tracers generally decrease with altitude. H 2 O 2 and CH 3 OOH * show maxima above the boundary layer at 2-5 km, being more distinct over southern than over northern Europe.We also present a comparison of our data with simulations by two global 3-D-models, MATCH-MPIC and EMAC, and with the box model CAABA. The models realistically represent altitude and latitude gradients for both HCHO and hydroperoxides (ROOH). In contrast, the models have problems reproducing the absolute mixing ratios, in particular of H 2 O 2 . Large uncertainties about retention coefficients and Correspondence to: H. Fischer (horst.fischer@mpic.de) cloud microphysical parameters suggest that cloud scavenging might be a large source of error for the simulation of H 2 O 2 . A sensitivity study with EMAC shows a strong influence of cloud and precipitation scavenging on the budget of H 2 O 2 as simulations improve significantly with this effect switched off.

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Section: Introductionsupporting

confidence: 52%

Distribution of hydrogen peroxide and formaldehyde over Central Europe during the HOOVER project

et al. 2011

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“…Notholt et al (1997); Rinsland et al (2002) and Zhao et al (2002) have all retrieved CO, C 2 H 6 and C 2 H 2 using ground based FTIRs (Fourier Transform Infrared Spectrometers) from solar and lunar measurements. Carbon monoxide concentrations from space have been obtained by many different instruments such as SCIAMACHY, MOPITT, and TES (Buchwitz et al, 2006;Deeter et al, 2003;Luo et al, 2007) that have a nadir viewing geometry and the ATMOS, MIPAS, SMR, ACE and MLS (Barret et al, 2006;Clerbaux et al, 2008;Funke et al, 2007;Rinsland et al, 2000;Pumphrey et al, 2007) instruments with a limb viewing geometry. Ethane concentrations have been retrieved previously by MIPAS and ACE (Glatthor et al, 2009; from enhanced concentrations in biomass burning plumes.…”

Section: Introductionmentioning

confidence: 99%

Ethane, ethyne and carbon monoxide concentrations in the upper troposphere and lower stratosphere from ACE and GEOS-Chem: a comparison study

et al. 2011

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Near global upper tropospheric concentrations of carbon monoxide (CO), ethane (C2H6) and ethyne (C2H2) from ACE (Atmospheric Chemistry Experiment) Fourier transform spectrometer on board the Canadian satellite SCISAT-1 are presented and compared with the output from the Chemical Transport Model (CTM) GEOS-Chem. The retrievals of ethane and ethyne from ACE have been improved for this paper by using new sets of microwindows compared with those for previous versions of ACE data. With the improved ethyne retrieval we have been able to produce a near global upper tropospheric distribution of C2H2 from space. Carbon monoxide, ethane and ethyne concentrations retrieved using ACE spectra show the expected seasonality linked to variations in the anthropogenic emissions and destruction rates as well as seasonal biomass burning activity. The GEOS-Chem model was run using the dicarbonyl chemistry suite, an extended chemical mechanism in which ethyne is treated explicitly. Seasonal cycles observed from satellite data are well reproduced by the model output, however the simulated CO concentrations are found to be systematically biased low over the Northern Hemisphere. An average negative global mean bias of 12% and 7% of the model relative to the satellite observations has been found for CO and C2H6 respectively and a positive global mean bias of 1% has been found for C2H2. ACE data are compared for validation purposes with MkIV spectrometer data and Global Tropospheric Experiment (GTE) TRACE-A campaign data showing good agreement with all of them

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“…The production rate of CO from methanol is essentially equivalent to the production rate of HCHO, since the HCHO lifetime is ∼10 times shorter than that of methanol (Atkinson et al, 2006), and depositional sinks for HCHO are small (Dufour et al, 2009). Figure 8 shows the CO and HCHO production rates computed from the methanol measurements at the KCMP tall tower.…”

Section: Methanol As a Source Of Hcho And Comentioning

confidence: 99%

Sources and seasonality of atmospheric methanol based on tall tower measurements in the US Upper Midwest

Millet

Möhr

et al. 2011

Atmos. Chem. Phys.

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Abstract. We present over one year (January 2010-February 2011 of continuous atmospheric methanol measurements from the University of Minnesota tall tower Trace Gas Observatory (KCMP tall tower; 244 m a.g.l.), and interpret the dataset in terms of constraints on regional methanol sources and seasonality. The seasonal cycle of methanol concentrations observed at the KCMP tall tower is generally similar to that simulated by a global 3-D chemical transport model (GEOS-Chem, driven with MEGANv2.0 biogenic emissions) except the seasonal peak occurs ∼1 month earlier in the observations, apparently reflecting a model underestimate of emission rates for younger versus older leaves. Based on a source tracer approach, which we evaluate using GEOS-Chem and with multiple tracers, we estimate that anthropogenic emissions account for approximately 40 % of ambient methanol abundance during winter and 10 % during summer. During daytime in summer, methanol concentrations increase exponentially with temperature, reflecting the temperature sensitivity of the biogenic source, and the observed temperature dependence is statistically consistent with that in the model. Nevertheless, summertime concentrations are underestimated by on average 35 % in the model for this region. The seasonal importance of methanol as a source of formaldehyde (HCHO) and carbon monoxide (CO) is highest in spring through early summer, when biogenic methanol emissions are high but isoprene emissions are still relatively low. During that time observed methanol concentrations account for on average 20 % of the total CO and HCHO production rates as simulated by GEOS-Chem, compared to 12 % later in the summer and 12 % on an annualCorrespondence to: D. B. Millet (dbm@umn.edu) average basis. The biased seasonality in the model means that the photochemical role for methanol early in the growing season is presently underestimated.

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Global upper-tropospheric formaldehyde: seasonal cycles observed by the ACE-FTS satellite instrument

Cited by 41 publications

References 71 publications

Distribution of hydrogen peroxide and formaldehyde over Central Europe during the HOOVER project

Distribution of hydrogen peroxide and formaldehyde over Central Europe during the HOOVER project

Ethane, ethyne and carbon monoxide concentrations in the upper troposphere and lower stratosphere from ACE and GEOS-Chem: a comparison study

Sources and seasonality of atmospheric methanol based on tall tower measurements in the US Upper Midwest

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