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

• Published in: Journal of Geophysical Research: Atmospheres
• Main Authors: Real, E., Law, K., Weinzierl, Bernadett, Fiebig, Monika, Petzold, Andreas, Wild, O., Methven, J., Arnold, S., Stohl, Andreas, Huntrieser, Heide, Roiger, Anke, Schlager, Hans, Stewart, D., Avery, M., Sachse, G., Browell, Edward, Ferrare, R., Blake, D.
• Format: Article in Journal/Newspaper
• Language: English
• Published: Wiley 2007
• Subjects: Atmosphärische Spurenstoffe; North Atlantic; Alaska
• Online Access: https://elib.dlr.de/45575/; https://elib.dlr.de/45575/1/2006JD007576.pdf; http://www.agu.org/journals/jd/jd0709/2006JD007576/2006JD007576.pdf

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 O3 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 O3 production and 24% in O3 destruction over 5 days when including aerosols. The plume is found to be chemically active with large O3 increases attributed primarily to PAN decomposition during descent of the plume toward Europe. The predicted O3 changes are very dependent on temperature changes during transport and also on water vapor levels in the lower troposphere which can lead to O3 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 O3/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 ...