References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-9-7623-2009

Closing the peroxy acetyl nitrate budget: observations of acyl peroxy nitrates (PAN, PPN, and MPAN) during BEARPEX 2007

LaFranchi

B. W.

¹ Wolfe

G. M.

² Thornton

J. A.

³ Harrold

S. A.

³ Browne

E. C.

¹ Min

K. E.

⁴ Wooldridge

P. J.

¹ Gilman

J. B.

⁵ Kuster

W. C.

⁵ Goldan

P. D.

⁵ de Gouw

J. A.

⁵ McKay

⁶ ⁸ Goldstein

A. H.

⁶ Ren

⁷ ⁹ Mao

⁷ ¹⁰ Cohen

R. C.

¹ ⁴

Department of Chemistry, University of California, Berkeley, Berkeley, CA, USA

Department of Chemistry, University of Washington, Seattle, WA, USA

Department of Atmospheric Sciences, University of Washington, Seattle, WA, USA

Department of Earth and Planetary Science, University of California, Berkeley, CA, USA

NOAA/ESRL Chemical Sciences Division, Boulder, CO, USA

Department of Environmental Science, Policy, and Management, University of California, Berkeley, Berkeley, CA, USA

Department of Meteorology, Penn State University, University Park, PA, USA

now at: California Air Resources Board, Sacramento, CA, USA

now at: Rubenstein School of Marine and Atmospheric Science, University of Miami, Miami, FL, USA

now at: School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, USA

12 10 2009

9 19 7623 7641

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/9/7623/2009/acp-9-7623-2009.html

The full text article is available as a PDF file from http://www.atmos-chem-phys.net/9/7623/2009/acp-9-7623-2009.pdf

Acyl peroxy nitrates (APNs, also known as PANs) are formed from the oxidation of aldehydes and other oxygenated VOC (oVOC) in the presence of NO2. There are both anthropogenic and biogenic oVOC precursors to APNs, but a detailed evaluation of this chemistry against observations has proven elusive. Here we describe measurements of PAN, PPN, and MPAN along with the majority of chemicals that participate in their production and loss, including OH, HO2, numerous oVOC, and NO2. Observations were made during the Biosphere Effects on AeRosols and Photochemistry Experiment (BEARPEX 2007) in the outflow of the Sacramento urban plume. These observations are used to evaluate a detailed chemical model of APN ratios and concentrations. We find that the ratios of APNs are nearly independent of the loss mechanisms and thus an especially good test of our understanding of their sources. We show that oxidation of methylvinyl ketone, methacrolein, methyl glyoxal, biacetyl and acetaldehyde are all significant sources of the PAN+peroxy acetyl (PA) radical reservoir, accounting for 26%, 2%, 7%, 20%, and 45%, of the production rate on average during the campaign, respectively. At high temperatures, when upwind isoprene emissions are highest, oxidation of non-acetaldehyde PA radical sources contributes over 60% to the total PA production rate, with methylvinyl ketone being the most important of the isoprene-derived sources. An analysis of absolute APN concentrations reveals a missing APN sink that can be resolved by increasing the PA+∑RO2 rate constant by a factor of 3.

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