References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-10-3405-2010

Global atmospheric budget of acetaldehyde: 3-D model analysis and constraints from in-situ and satellite observations

Millet

D. B.

¹ Guenther

² Siegel

D. A.

³ Nelson

N. B.

³ Singh

H. B.

⁴ de Gouw

J. A.

⁵ Warneke

⁵ Williams

⁶ Eerdekens

⁶ Sinha

⁶ Karl

² Flocke

² Apel

² Riemer

D. D.

⁷ Palmer

P. I.

⁸ Barkley

⁸

University of Minnesota, Department of Soil, Water and Climate, St. Paul, Minnesota, USA

NCAR, Atmospheric Chemistry Division, Boulder, Colorado, USA

University of California, Santa Barbara, Institute for Computational Earth System Science, Santa Barbara, California, USA

NASA Ames Research Center, Moffett Field, California, USA

NOAA ESRL, Boulder, Colorado, USA

Max Planck Institute for Chemistry, Mainz, Germany

University of Miami, Rosenstiel School of Marine and Atmospheric Science, Miami, Florida, USA

University of Edinburgh, School of GeoSciences, Edinburgh, UK

12 04 2010

10 7 3405 3425

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.

This article is available from http://www.atmos-chem-phys.net/10/3405/2010/acp-10-3405-2010.html

The full text article is available as a PDF file from http://www.atmos-chem-phys.net/10/3405/2010/acp-10-3405-2010.pdf

We construct a global atmospheric budget for acetaldehyde using a 3-D model of atmospheric chemistry (GEOS-Chem), and use an ensemble of observations to evaluate present understanding of its sources and sinks. Hydrocarbon oxidation provides the largest acetaldehyde source in the model (128 Tg a−1, a factor of 4 greater than the previous estimate), with alkanes, alkenes, and ethanol the main precursors. There is also a minor source from isoprene oxidation. We use an updated chemical mechanism for GEOS-Chem, and photochemical acetaldehyde yields are consistent with the Master Chemical Mechanism. We present a new approach to quantifying the acetaldehyde air-sea flux based on the global distribution of light absorption due to colored dissolved organic matter (CDOM) derived from satellite ocean color observations. The resulting net ocean emission is 57 Tg a−1, the second largest global source of acetaldehyde. A key uncertainty is the acetaldehyde turnover time in the ocean mixed layer, with quantitative model evaluation over the ocean complicated by known measurement artifacts in clean air. Simulated concentrations in surface air over the ocean generally agree well with aircraft measurements, though the model tends to overestimate the vertical gradient. PAN:NOx ratios are well-simulated in the marine boundary layer, providing some support for the modeled ocean source. We introduce the Model of Emissions of Gases and Aerosols from Nature (MEGANv2.1) for acetaldehyde and ethanol and use it to quantify their net flux from living terrestrial plants. Including emissions from decaying plants the total direct acetaldehyde source from the land biosphere is 23 Tg a−1. Other terrestrial acetaldehyde sources include biomass burning (3 Tg a−1) and anthropogenic emissions (2 Tg a−1). Simulated concentrations in the continental boundary layer are generally unbiased and capture the spatial gradients seen in observations over North America, Europe, and tropical South America. However, the model underestimates acetaldehyde levels in urban outflow, suggesting a missing source in polluted air. Ubiquitous high measured concentrations in the free troposphere are not captured by the model, and based on present understanding are not consistent with concurrent measurements of PAN and NOx: we find no compelling evidence for a widespread missing acetaldehyde source in the free troposphere. We estimate the current US source of ethanol and acetaldehyde (primary + secondary) at 1.3 Tg a−1 and 7.8 Tg a−1, approximately 60{%} and 480% of the corresponding increases expected for a national transition from gasoline to ethanol fuel.

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