Processes influencing ozone levels in Alaskan forest fire plumes during long-range transport over the North Atlantic

被引:132
作者
Real, E.
Law, K. S.
Weinzierl, B.
Fiebig, M.
Petzold, A.
Wild, O.
Methven, J.
Arnold, S.
Stohl, A.
Huntrieser, H.
Roiger, A.
Schlager, H.
Stewart, D.
Avery, M.
Sachse, G.
Browell, E.
Ferrare, R.
Blake, D.
机构
[1] Univ Paris 06, Inst Pierre Simon Laplace, CNRS, Serv Aeron, F-75005 Paris, France
[2] Deutsch Zentrum Luft & Raumfahrt, Inst Phys Atmosphare, D-82230 Wessling, Germany
[3] Univ Cambridge, Dept Chem, Ctr Atmospher Sci, Cambridge CB2 1EW, England
[4] Univ Reading, Dept Meteorol, Reading RG6 6BB, Berks, England
[5] Univ Leeds, Sch Earth & Environm, Leeds LS2 9JT, W Yorkshire, England
[6] Norwegian Inst Air Res, N-2027 Kjeller, Norway
[7] Univ E Anglia, Sch Environm Sci, Norwich NR4 7TJ, Norfolk, England
[8] NASA, Div Atmospher Sci, Langley Res Ctr, Hampton, VA 23681 USA
[9] Univ Calif Irvine, Dept Chem, Irvine, CA 92697 USA
基金
英国自然环境研究理事会;
关键词
BIOMASS-BURNING EMISSIONS; TROPICAL SOUTH-ATLANTIC; OPTICAL-PROPERTIES; ATMOSPHERIC CHEMISTRY; UNITED-STATES; MODEL; AEROSOL; SUMMER; IMPACT; O-3;
D O I
10.1029/2006JD007576
中图分类号
P4 [大气科学(气象学)];
学科分类号
0706 ; 070601 ;
摘要
[1] A case of long-range transport of a biomass burning plume from Alaska to Europe is analyzed using a Lagrangian approach. This plume was sampled several times in the free troposphere over North America, the North Atlantic and Europe by three different aircraft during the IGAC Lagrangian 2K4 experiment which was part of the ICARTT/ ITOP measurement intensive in summer 2004. Measurements in the plume showed enhanced values of CO, VOCs and NOy, mainly in form of PAN. Observed O-3 levels increased by 17 ppbv over 5 days. A photochemical trajectory model, CiTTyCAT, was used to examine processes responsible for the chemical evolution of the plume. The model was initialized with upwind data and compared with downwind measurements. The influence of high aerosol loading on photolysis rates in the plume was investigated using in situ aerosol measurements in the plume and lidar retrievals of optical depth as input into a photolysis code (Fast-J), run in the model. Significant impacts on photochemistry are found with a decrease of 18% in O-3 production and 24% in O-3 destruction over 5 days when including aerosols. The plume is found to be chemically active with large O-3 increases attributed primarily to PAN decomposition during descent of the plume toward Europe. The predicted O-3 changes are very dependent on temperature changes during transport and also on water vapor levels in the lower troposphere which can lead to O-3 destruction. Simulation of mixing/dilution was necessary to reproduce observed pollutant levels in the plume. Mixing was simulated using background concentrations from measurements in air masses in close proximity to the plume, and mixing timescales ( averaging 6.25 days) were derived from CO changes. Observed and simulated O-3/CO correlations in the plume were also compared in order to evaluate the photochemistry in the model. Observed slopes change from negative to positive over 5 days. This change, which can be attributed largely to photochemistry, is well reproduced by multiple model runs even if slope values are slightly underestimated suggesting a small underestimation in modeled photochemical O-3 production. The possible impact of this biomass burning plume on O-3 levels in the European boundary layer was also examined by running the model for a further 5 days and comparing with data collected at surface sites, such as Jungfraujoch, which showed small O-3 increases and elevated CO levels. The model predicts significant changes in O-3 over the entire 10 day period due to photochemistry but the signal is largely lost because of the effects of dilution. However, measurements in several other BB plumes over Europe show that O-3 impact of Alaskan fires can be potentially significant over Europe.
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页数:19
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