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The Cambridge Tropospheric Trajectory model of Chemistry and Transport (CiTTyCAT), a Lagrangian chemistry model, has burn evaluated using atmospheric chemical measurements collected during the East Atlantic Summer Experiment 1996 (EASE '96), This field campaign was part of the UK Natural Environment Research Council's (NERC) Atmospheric Chemistry Studies in the Oceanic Environment (ACSOE) programme, conducted at Mace Head, Republic of Ireland, during July and August 1996. The model includes a description of gas-phase tropospheric chemistry, and simple parameterisations for surface deposition, mixing from the free troposphere and emissions. The model generally compares well with the measurements and is used to study the production and loss of O-3 under a variety of conditions. The mean difference between the hourly O-3 concentrations calculated by the model and those measured is 0.6 ppbv with a standard deviation of 8.7 ppbv. Three specific air-flow regimes were identified during the campaign - westerly, anticyclonic (easterly) and south westerly. The westerly how is typical of background conditions for Mace Head. However, on some occasions there was evidence of long-range transport of pollutants from North America. In periods of anticyclonic flow, air parcels had collected emissions of NOx and VOCs immediately before arriving at Mace Head, leading to O-3 production. The level of calculated O-3 depends critically on the precise details of the trajectory, and hence on the emissions into the air parcel. In several periods of south westerly flow, low concentrations of O-3 were measured which were consistent with deposition and photochemical destruction inside the tropical marine boundary layer. (C) 2000 Elsevier Science Ltd. All rights reserved.

A Lagrangian photochemical trajectory model has been used to assess the factors affecting O-3 production during transport of polluted air masses across the North Atlantic Ocean. Sensitivity studies have been performed along idealized trajectories, and it is found that the potential impact of North American emission sources is maximized by transport of air at high altitudes, in drier conditions and in conditions where mixing of the air with background air masses is relatively limited. Measurements taken from the NCAR King Air aircraft as part of the North Atlantic Regional Experiment (NARE) August 1993 intensive have been used to initialize forward trajectories, calculated using European Centre for Medium-Range Weather Forecasting analyzed wind fields, from eastern North America to assess O-3 production over the Atlantic during this period. The effects of dilution of a polluted air parcel with air from the upper troposphere have also been studied, and the contribution of photochemical O-3 production to the air mass composition is found to be smaller than that of dilution, particularly for long trajectories and for conditions where dilution is relatively rapid or involves air from the stratosphere. Measurements taken from the Meteorological Research Flight Hercules aircraft over the eastern Atlantic as part of the Oxidizing Capacity of the Tropospheric Atmosphere campaign have been examined in the light of these studies. A backward trajectory analysis has been performed from one of the vertical profiles taken off the coast of Portugal on August 31, 1993, to assess the origin of the different air masses intercepted. While the lower levels are characteristic of air from the European boundary layer advected over the ocean, the upper levels show strong evidence for anthropogenic influence from North American sources, with elevated levels of O-3, NOy, CO, and aerosol. Although it cannot be concluded that this air mass definitely originated from over North America, the meas