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Volume 16, issue 5
Atmos. Chem. Phys., 16, 3485–3497, 2016
https://doi.org/10.5194/acp-16-3485-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.

Special issue: Quantifying the impact of Boreal fires on tropospheric oxidants...

Atmos. Chem. Phys., 16, 3485–3497, 2016
https://doi.org/10.5194/acp-16-3485-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.

Research article 17 Mar 2016

Research article | 17 Mar 2016

Production of peroxy nitrates in boreal biomass burning plumes over Canada during the BORTAS campaign

Marcella Busilacchio1, Piero Di Carlo1,2, Eleonora Aruffo1,2, Fabio Biancofiore1,2, Cesare Dari Salisburgo1, Franco Giammaria2, Stephane Bauguitte3, James Lee4, Sarah Moller4, James Hopkins4, Shalini Punjabi4, Stephen Andrews4, Alistair C. Lewis4, Mark Parrington5,a, Paul I. Palmer5, Edward Hyer6, and Glenn M. Wolfe7,8 Marcella Busilacchio et al.
  • 1Center of Excellence CETEMPS, University of L'Aquila, Via Vetoio, Coppito, L'Aquila, Italy
  • 2Department of Physical and Chemical Sciences, University of L'Aquila, Coppito, L'Aquila, Italy
  • 3Facility for Airborne Atmospheric Measurements, Bedfordshire, UK
  • 4Department of Chemistry, University of York, York, UK
  • 5School of GeoSciences, University of Edinburgh, Edinburgh, UK
  • 6Marine Meteorology Division, Naval Research Laboratory, Monterey, California, USA
  • 7Atmospheric Chemistry and Dynamics Laboratory, NASA Goddard Space Flight Center, Greenbelt, Maryland, USA
  • 8Joint Center for Earth Systems Technology, University of Maryland Baltimore County, Baltimore, MD, USA
  • anow at: European Centre for Medium-Range Weather Forecasts (ECMWF), Reading, UK

Abstract. The observations collected during the BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites (BORTAS) campaign in summer 2011 over Canada are analysed to study the impact of forest fire emissions on the formation of ozone (O3) and total peroxy nitrates ∑PNs, ∑ROONO2). The suite of measurements on board the BAe-146 aircraft, deployed in this campaign, allows us to calculate the production of O3 and of  ∑PNs, a long-lived NOx reservoir whose concentration is supposed to be impacted by biomass burning emissions. In fire plumes, profiles of carbon monoxide (CO), which is a well-established tracer of pyrogenic emission, show concentration enhancements that are in strong correspondence with a significant increase of concentrations of ∑PNs, whereas minimal increase of the concentrations of O3 and NO2 is observed. The ∑PN and O3 productions have been calculated using the rate constants of the first- and second-order reactions of volatile organic compound (VOC) oxidation. The ∑PN and O3 productions have also been quantified by 0-D model simulation based on the Master Chemical Mechanism. Both methods show that in fire plumes the average production of ∑PNs and O3 are greater than in the background plumes, but the increase of ∑PN production is more pronounced than the O3 production. The average ∑PN production in fire plumes is from 7 to 12 times greater than in the background, whereas the average O3 production in fire plumes is from 2 to 5 times greater than in the background. These results suggest that, at least for boreal forest fires and for the measurements recorded during the BORTAS campaign, fire emissions impact both the oxidized NOy and O3,  but (1 ∑PN production is amplified significantly more than O3 production and (2) in the forest fire plumes the ratio between the O3 production and the ∑PN production is lower than the ratio evaluated in the background air masses, thus confirming that the role played by the ∑PNs produced during biomass burning is significant in the O3 budget. The implication of these observations is that fire emissions in some cases, for example boreal forest fires and in the conditions reported here, may influence more long-lived precursors of O3 than short-lived pollutants, which in turn can be transported and eventually diluted in a wide area.

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Boreal fire emissions have little effect on ozone concentrations but evident impact on some NOx reservoirs as peroxy nitrates that we quantified. This should be taken into account since NOx reservoirs can be efficiently transported and may influence the ozone budget far away from the fire emission. The study is based on observations carried out on board the BAe 146 aircraft during BORTAS in Canada. We used a custom laser-induced fluorescence system to measure NO2 and NOx reservoirs.
Boreal fire emissions have little effect on ozone concentrations but evident impact on some NOx...
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