Tropospheric ozone: The role of transport

Abstract

The Geophysical Fluid Dynamics Laboratory general circulation/transport model, with photochemistry in the top level (middle stratosphere) only, is used to simulate global tropospheric ozone distributions for upper and lower limits of surface removal rates. We compared these simulations with available observations and find that large‐scale atmospheric transport plays a major role in the behavior of tropospheric ozone. Furthermore, we identify potential roles for tropospheric chemistry, discover defects in the model's simulations of transport, and gain a more global picture of tropospheric ozone. The transport model's mean cross‐tropopause flux is in the range of previous estimates, and the shapes of the simulated vertical profiles of mixing ratio and percent standard deviation are in good agreement with observations. South of 40°N, the simulated and observed latitude gradients are the same, the upper and lower limit calculations bracket measured values, and the seasonal cycles are well reproduced. While the transport model simulates a wide range of tropospheric ozone climatology, there are a significant number of disagreements. The need for additional ozone destruction in the maritime boundary layer suggests a role for chemical destruction, while in the continental boundary layer, it appears that chemical production, a seasonal cycle in surface deposition, and improved boundary layer transport are all required. The two major defects in the simulated “free troposphere” are (1) excess ozone at high latitudes of the northern hemisphere (NH) and (2) spring rather than summer maxima and fall rather than winter minima at NH mid‐ and high latitudes. While defect 1 has a number of possible causes, deficiencies in model transport play a major role. Although similar transport defects have not been ruled out for defect 2, tropospheric chemistry appears to be needed. Separate calculations of the net chemical production and loss demonstrate that this is a complex problem. The most likely solution involves the transport control of NOx which controls the ozone chemistry.