References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-9-1647-2009

SCIAMACHY formaldehyde observations: constraint for isoprene emission estimates over Europe?

Dufour

¹ Wittrock

² Camredon

¹ ³ Beekmann

¹ Richter

² Aumont

¹ Burrows

J. P.

Laboratoire Inter-universitaire des Systèmes Atmosphériques (LISA), UMR7583, Universités Paris 12 et Paris 7, CNRS, Créteil, France

Institute of Environmental Physics and Remote Sensing, University of Bremen, Bremen, Germany

now at: School of Geography, Earth and Environment Sciences, University of Birmingham, Edgbaston, Birmingham, UK

05 03 2009

9 5 1647 1664

This is an open-access article ditributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited.

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Formaldehyde (HCHO) is an important intermediate compound in the degradation of volatile organic compounds (VOCs) in the troposphere. Sources of HCHO are largely dominated by its secondary production from VOC oxidation, methane and isoprene being the main precursors in unpolluted areas. As a result of the moderate lifetime of HCHO, its spatial distribution is determined by reactive hydrocarbon emissions. We focus here on Europe and investigate the influence of the different emissions on HCHO tropospheric columns with the CHIMERE chemical transport model in order to interpret the comparisons between SCIAMACHY and simulated HCHO columns. Europe was never specifically studied before for these purposes using satellite observations. The bias between measurements and model is less than 20% on average. The differences are discussed according to the errors on the model and the observations and remaining discrepancies are attributed to a misrepresentation of biogenic emissions. This study requires the characterisation of: (1) the model errors and performances concerning formaldehyde. The errors on the HCHO columns, mainly related to chemistry and mixed emission types, are evaluated to 2×1015 molecule/cm2 and the model performances evaluated using surface measurements are satisfactory (~13%); (2) the observation errors that define the needs in spatial and temporal averaging for meaningful comparisons. Using SCIAMACHY observations as constraint for biogenic isoprene emissions in an inverse modelling scheme reduces their uncertainties by about a factor of two in region of intense emissions. The retrieved correction factors for the isoprene emissions range from a factor of 0.15 (North Africa) to a factor of 2 (Poland, the United Kingdom) depending on the regions.

References 1

Abbot, D. S., Palmer, P. I., Martin, R. V., Chance, K., Jacob, D. J., and Guenther, A.: Seasonal and interannual variability of North American isoprene emissions as determined by formaldehyde column measurements from space, Geophys. Res. Lett., 30(17), 1886, doi:10.1029/2003GL017336, 2003.

Atkinson, R.: Gas-phase tropospheric chemistry of organic compounds, J. Phys. Chem. Ref. Data Monogr., 2, 13–46, 1994.

Aumont, B., Szopa, S., and Madronich, S.: Modelling the evolution of organic carbon during its gas-phase tropospheric oxidation: development of an explicit model based on a self generating approach, Atmos. Chem. Phys., 5, 2497–2517, 2005.

Beekmann, M. and Derognat, C.: Monte Carlo uncertainty analysis of a regional-scale transport chemistry model constrained by measurements from the Atmospheric Pollution Over the Paris Area (ESQUIF) campaign, J. Geophys. Res., 108(D17), 8559, doi:10.1029/2003JD003391, 2003.

Bessagnet, B., Hodzic, A., Vautard, R., Beekmann, M., Cheinet, S., Honor, C., Liousse, C., and Rouil, L.: Aerosol modeling with CHIMERE – Preliminary evaluation at the continentale scale, Atmos. Environ., 38, 2803–2817, 2004.

Blond, N., Bel., L., and Vautard, R.: Three-dimensional ozone dara analysis with an air quality model over the Paris area, J. Geophys. Res., 108(D23), 4744, doi:10.1029/2003JD003679, 2003.

Blond, N. and Vautard, N.: Three-dimensional ozone analyses and their use for short-term ozone forecasts, J. Geophys. Res., 109, D17303, doi:10.1029/2004JD004515, 2004.

Blond, N., Boersma, K. F., Eskes, H. J., van der A, R. J., Van Roozendeal, M., De Smedt, I., Bergametti, G., and Vautard, R.: Intercomparison of SCIAMACHY nitrogen dioxide observations, in situ measurements and air quality modeling results over Western Europe, J. Geophys. Res., 112, D10311, doi:10.1029/2006JD007277, 2007.

Boissard, C., Chervier, F., and Dutot, A. L.: Assessment of high (diurnal) to low (seasonal) frequency variations of isoprene emission rates using a neural network approach, Atmos. Chem. Phys., 8, 2089–2101, 2008.

Bovensmann, H., Burrows, J. P., Buchwitz, M., Frerick, J., No\"el, S., Rozanov, V., Chance, K., and Goede, A. H. P.: SCIAMACHY: mission objectives and measurement modes, J. Atmos. Sci., 56, 127–150, 1999.

Carter, W. P. L.: Documentation of the SAPRC-99 chemical mechanism for the VOC reactivity assessment, Final Report to the California Air Resources Board under Contracts 92-329 and 95-308, Center of Environmental Research and Technology, Riverside, http://www.engr.ucr.edu/~carter/absts.htm#saprc99, 2000.

Camredon,~M., Aumont,~B., Lee-Taylor,~J., and Madronich,~S.: The SOA/VOC/NOx system: an explicit model of secondary organic aerosol formation, Atmos. Chem. Phys., 7, 5599–5610, 2007.

Chance,~K., Palmer,~P. I., Spurr,~R. J. D., Martin,~R. V., Kurosu, T. P., and Jacob, D.: Satellite observations of formaldehyde over North America from GOME, Geophys. Res. Lett., 27, 3461–3464, 2000.

Curci, G., Beekmann, M., Vautard, R., Smiatek, G., Steinbrecher, R., Theloke, J., and Friedrich, R.: Modelling study of the impact of isoprene and terpene biogenic emissions on European ozone levels, Atmos. Environ., 43, 1444–1455, 2009.

Deguillaume, L., Beekmann, M., and Menut, L.: Bayesian Monte Carlo analysis applied to regional-scale inverse emission modeling for reactive trace gases, J. Geophys. Res., 112, D02307, doi:10.1029/2006JD007518, 2007.

De Smedt, I., Müller, J.-F., Stavrakou, T., van der A, R., Eskes, H., and Van Roozendael, M.: Twelve years of global observations of formaldehyde in the troposphere using GOME and SCIAMACHY sensors, Atmos. Chem. Phys., 8, 4947–4963, 2008.

Friedrich, R.: GENEMIS: Assessment, improvement, temporal and spatial disaggregation of European emission data, in: Tropospheric Modelling and Emission Estimation, part 2, edited by: Ebel, A., Friedrich, R., and Rhode, H., 181–214, Springer, New-York, 1997.

Fu, T., Jacob, D. J., Palmer, P. I., Chance, K., Wang, Y. X., Barletta, B., Blake, D. R., Stanton, J. C., and Pilling, M. J.: Space-based formaldehyde measurements as constraints on volatile organic compound emissions is east and south Asia and implications for ozone, J. Geophys. Res., 112, D06312, doi:10.1029/2006JD007853, 2007.

Guenther, A., Hewitt, C. N., Erickson, D., Fall, R., Geron, C., Graedel, T., Harley, P., Klinger, L., Lerdau, M., McKay, W. A., Pierce, T., Scholes, B., Steinbrecher, R., Tallamraju, R., Taylor, J., and Zimmerman, P.: A global model of natural volatile organic compound emissions, J. Geophys. Res., 100, 8873–8892, 1995.

Guenther, A., Karl, T., Harley, P., Wiedinmyer, C., Palmer, P. I., and Geron, C.: Estimates of global terrestrial isoprene emissions using MEGAN (Model of Emissions of Gases and Aerosols from Nature), Atmos. Chem. Phys., 6, 3181–3210, 2006.

Granier, C., Lamarque, J. F., Mieville, A., Muller, J. F., Olivier, J., Orlando, J., Peters, J., Petron, G., Tyndall, G., and Wallens, S.: POET, a database of surface emissions of ozone precursors, available on internet at http://www.aero.jussieu.fr/projet/ACCENT/POET.php, 2005.

Hauglustaine, D. A., Hourdin, F., Jourdain, L., Filiberti, M.-A., Walters, S., Lamarque, J.-F., and Holland, E. A.: Interactive chemistry in the Laboratoire de Météorologie Dynamique general circulation model: Description and background tropospheric chemistry evaluation, J. Geophys. Res., 109, D04314, doi:10.1029/2003JD003957, 2004.

Honoré C., Rou\"ıl, L., Vautard, R., Beekmann, M., Bessagnet, B., Dufour, A., Elichegaray, C., Flaud, J.-M., Malherbe, L., Meleux, F., Menut, L., Martin, D., Peuch, A., Peuch, V. H., and Poisson, N.: Predictability of European air quality: The assessment of three years of operational forecasts and analyses by the PREV'AIR system, J. Geophys. Res., D113, D04301, doi:10.1029/2007JD008761, 2008.

Horowitz, L. W., Walters, S., Mauzerall, D. L., et al.: A global simulation of tropospheric ozone and related tracers: Description and evaluation of MOZART, version 2, J. Geophys. Res., 108(D24), 4784, doi:10.1029/2002JD002853, 2003.

Jenkin, M. E., Saunders, S. M., Wagner, V., and Pilling, M. J.: Protocol for the development of the Master Chemical Mechanism, MCM v3 (Part B): tropospheric degradation of aromatic volatile organic compounds, Atmos. Chem. Phys., 3, 181–193, 2003.

Konovalov, I. B., Beekmann, M., Richter, A., and Burrows, J. P.: Inverse modelling of the spatial distribution of NOx emissions on a continental scale using satellite data, Atmos. Chem. Phys., 6, 1747–1770, 2006.

Konovalov, I. B., Beekmann, M., Burrows, J. P., and Richter, A.: Satellite measurement based estimates of decadal changes in European nitrogen oxides emissions, Atmos. Chem. Phys., 8, 2623–2641, 2008.

Lathière, J., Hauglustaine, D. A., Friend, A. D., De Noblet-Ducoudré, N., Viovy, N., and Folberth, G. A.: Impact of climate variability and land use changes on global biogenic volatile organic compound emissions, Atmos. Chem. Phys., 6, 2129–2146, 2006.

Lattuati, M.: Contribution à l'étude du bilan de l'ozone troposphérique à l'interface de l'Europe et de l'Atlantique Nord: Modélisation lagrangienne et mesures en altitude, PhD thesis, Université Paris 6, Paris, 1997.

Mandrovich, S. and Flocke, S.: The role of solar radiation in atmospheric chemistry, in: Handbook of Environmental Chemistry, edited by: Boule, P., Springer, New York, 1–26, 1998.

Menut, L., Vautard, R., Flamant, C., Abonnel, C., Beekmann, M., Chazette, P., Flamant, P. H., Gombert, D., Guédalia, D., Kley, D., Lefebvre, M. P., Lossec, B., Martin, D., Mégie, G., Perros, P., Sicard, M., and Toupance, G.: Measurements and modelling of atmospheric pollution over the Paris area: An overview of the ESQUIF project, Ann. Geophys., 18, 1467–1481, 2000.

Menut, L.: Adjoint modelling for atmospheric pollution process sensitivity at regional scale, J. Geophys. Res., 108(D17), 8562, doi:10.1029/2002JD002549, 2003.

Meyer-Arnek, J., Ladstätter-Weißenmayer, Richter, A., Wittrock, F., and Buurows, J. P.: A study of the trace gas columns of O3, NO2, and HCHO over Africa in September 1997, Faraday Discuss., 130, 387–405, 2005.

Middleton, P., Stockwell, W. R., and Carter, W. P.: Aggregation and analysis of volatile organic compound emissions for regional modelling, Atmos. Environ., 24, 1107–1133, 1990.

Millet, D. B., Jacob, D. J., Boersma, K. F., Fu, T., Kurosu, T. P., Chance, K., Heald, C. L., and Guenther, A.: Spatial distribution of isoprene emissions from North America derived from formaldehyde column measurements by the OMI satellite sensor, J. Geophys. Res., 113, D02307, doi:10.1029/2007JD008950, 2008.

Müller, J.-F., Stavrakou, T., Wallens, S., De Smedt, I., Van Roozendael, M., Potosnak, M. J., Rinne, J., Munger, B., Goldstein, A., and Guenther, A. B.: Global isoprene emissions estimated using MEGAN, ECMWF analyses and a detailed canopy environment model, Atmos. Chem. Phys., 8, 1329–1341, 2008.

Palmer, P. I., Jacob, D. J., Chance, K., Martin, R. V., Spurr, R. J. D., Kurosu, T. P., Bey, I., Yantosca, R., Fiore, A., and Li, Q.: Air mass factor formulation for spectroscopic measurements from satellites: Application to formaldehyde retrievals from the Global Ozone Monitoring Experiment, J. Geophys. Res., 106(D13), 14539–14550, 2001.

Palmer, P. I., Jacob, D. J., Fiore, A. M., Martin, R. V., Chance, K., and Kurosu, T. P.: Mapping isoprene emissions over North America using formaldehyde column observations from space, J. Geophys. Res., 108(D6), 4180, doi:10.1029/2002JD002153, 2003.

Palmer, P. I., Abbot, D. S., Fu, T., Jacob, D. J., Chance, K., Kurosu, T. P., Guenther, A., Wiedinmyer, C., Stanton, J. C., Pilling, M. J., Pressley, S. N., Lamb, B., and Sumner, A. L.: Quantifying the seasonal and interannual variability of North American isoprene emissions using satellite observations of the formaldehyde column, J. Geophys. Res., 11, D12315, doi:10.1029/2005JD006689, 2006.

Pfister, G. G., Emmons, L. K., Hess, P. G., Lamarque, J.-F., Orlando, J. J., Walters, S., Guenther, A., Palmer, P. I., and Lawrence, P. J.: Contribution of isoprene to chemical budgets: A model tracer study with the NCAR CTM MOZART-4, J. Geophys. Res., 113, D05308, doi:10.1029/2007JD008948, 2008.

Pison, I., Menut, L., and Bergametti, G.: Inverse modeling of surface NOx anthropogenic emission fluxes in the Paris area during the air pollution over Paris Region (ESQUIF) campaign, J. Geophys. Res., 112, D24302, doi:10.1029/2007JD008871, 2007.

Richter, A. and Burrows, J. P.: Tropospheric NO2 from GOME measurements, Adv. Space Res., 29, 1673–1683, 2002.

Rodgers, C. D.: Inverse Methods for Atmospheric Sounding: Theory and Practice, World Sci., Hackensack, N.J, 2000.

Saunders, S. M., Jenkin, M. E., Derwent, R. G., and Pilling, M. J.: Protocol for the development of the Master Chemical Mechanism, MCM v3 (Part A): tropospheric degradation of \mboxnon-aromatic volatile organic compounds, Atmos. Chem. Phys., 3, 161–180, 2003.

Schmidt, H., Derognat, C., Vautard, R., and Beekmann, M.: A comparison of simulated and observed ozone mixing ratios for summer of 1998 in western Europe, Atmos. Environ., 35, 6277–6297, 2001.

Shim, C., Wang, Y., Choi, Y., Palmer, P. I., Abbot, D. S., and Chance, K.: Constraining global isoprene emissions with Global Ozone Monitoring Experiment (GOME) formaldehyde column measurements, J. Geophys. Res., 110, D24301, doi:10.1029/2004JD005629, 2005.

Simpson, D., Winiwater, W., Borjesson, G., Cinderby, S., Ferreiro, A., Guenther, A., Hewitt, C. N., Janson, R., Khalil, M. A. K., Oen, S., Svennson, B. H., Tarrason, L., and Oquist, M. G., J. Geophys. Res., 104, 8113–8152, 1999.

Solberg, S., Dye, C., Scmidbauer, N., and Simpson, D.: Evaluation of the VOC measurement programme within EMEP, NILU:EMEP/CCC-Report 5/95, ref. O-8852, June 1995.

Solberg, S., Coddeville, P., Dye, C., Honzàk, J., and Scmidbauer, N.: VOC measurements 1997, NILU:EMEP/CCC-Report 4/08, ref. O-92016, August 1998.

Solberg, S., Dye, C., Roemer, M., and Schmidbauer, N.: VOC measurements 1999, NILU:EMEP/CCC-Report 7/2001, ref. O-92016, July 2001, 2001a.

Solberg, S., Dye, C., Walker, S. E., and Simpson, D.: Long-term measurements and model calculations of formaldehyde at rural European monitoring sites, Atmos. Environ., 35, 195–207, 2001b.

Solberg, S.: VOC measurememts 2003, NILU:EMEP/CCC-Report 10/2005, ref. O-92016, August 2005. %

%Stavrakou, T., Müller, J.-F., De Smedt, I., Van Roozendael, M., van der Werf, %G. R., Giglio, L., and Guenther, A.: Evaluating the performance of pyrogenic %and biogenic emission inventories against one decade of space-based formaldehyde %columns, Atmos. Chem. Phys. Discuss., 8, 16981–17036, 2008.

Stavrakou, T., Müller, J.-F., De Smedt, I., Van Roozendael, M., van der Werf, G. R., Giglio, L., and Guenther, A.: Evaluating the performance of pyrogenic and biogenic emission inventories against one decade of space-based formaldehyde columns, Atmos. Chem. Phys., 9, 1037–1060, 2009.

Stohl, A., Williams, E., Wotawa, G., and Kromp-Kolb, H.: A European inventory of soil nitric oxide emissions and the effect of these emissions on the photochemical formation of ozone, Atmos. Environ., 30, 3741–3755, 1996.

Steinbrecher, R, Smiatek, G., Köble, R, Seufert, G., Theloke, J. Hauff, K., Ciccioli, P., Vautard, R., and Curci, G. : Intra- and inter-annual variability of VOC emissions from natural and semi-natural vegetation in Europe and neighbouring countries, Atmos. Environ., 43, 1380–1391, 2009.

Tiedtke, M.: A comprehensive mass flux scheme for cumulus parametrization in large-scale models, Mon. Weather Rev., 117, 1779–1800, 1989.

Tressol, M., Ordonez, C., Zbinden, R., Brioude, J., Thouret, V., Mari, C., Nedelec, P., Cammas, J.-P., Smit, H., Patz, H.-W., and Volz-Thomas, A.: Air pollution during the 2003 European heat wave as seen by MOZAIC airliners, Atmos. Chem. Phys., 8, 2133–2150, 2008.

Vautard, R., Beekmann, M., Roux, J., and Gombert, D.: Validation of a hybrid forecasting system for the ozone concentrations over the Paris area, Atmos. Environ., 35, 2449–2461, 2001.

Vautard, R., Martin, D., Beekmann, M., et al.: Paris emission inventory diagnostics from ESQUIF airborne measurements and a chemistry transport model, J. Geophys. Res., 108(D17), 8564, doi:10.1029/2002JD002797, 2003.

Vautard, R., Szopa, S., Beekmann, M., Menut, L., Hauglustaine, D. A., Rouil, L., and Roemer, M.: Are decadal anthropogenic emission reductions in Europe consistent with surface ozone observations?, Geophys. Res. Lett., 33, L13810, doi:10.1029/2006GL26080, 2006.

Vestreng, V., Adams, M., and Goodwin, J.: Inventory review 2004, Emission Data reported to CLRTAP and under the NEC Directive, EMEP/EEA Joint Review Report, EMEP/MSC-W Note 1/2004, ISSN 0804-2446, 2004.

Wittrock, F.: The retrieval of oxygenated volatile organic compounds by remote sensing techniques. Institute of Environmental Physics. Bremen: University of Bremen, 192, http://nbn-resolving.de/urn:nbn:de:gbv:46-diss000104818, 2006.

Wittrock, F., Richter, A., Ladstätter-Weißenmayer, A., and Burrows, J. P.: Global Observations of Formaldehyde, ERS-ENVISAT symposium, ESA, Gothenburg, http://earth.esa.int/pub/ESA_DOC/gothenburg/238wittr.pdf., 2000.

Wittrock, F., Richter, A., Oetjen, H., Burrows, J. P., Kanakidou, M., Myriokefalitakis, S., Volkmer, R., Beirle, S., Platt, U., and Wagner, T.: Simultaneous global observations of glyoxal and formaldehyde from space, Geophys. Res. Lett., 33, L16804, doi:10.1029/2006GL026310, 2006.