Date of Award

Spring 1-1-2013

Document Type

Dissertation

Degree Name

Doctor of Philosophy (PhD)

Department

Atmospheric & Oceanic Sciences

First Advisor

David C. Noone

Second Advisor

Mary C. Barth

Third Advisor

Darin Toohey

Fourth Advisor

William Skamarock

Fifth Advisor

Jana Milford

Abstract

Upper tropospheric ozone has significant impacts on the total atmospheric chemistry and radiative budget. Previous studies noted an upper tropospheric ozone enhancement above southern United States during the North Ameican Monsoon (NAM). This recurring phenomenon has been observed by the satellite-borne Tropospheric Emission Spectrometer (TES) and IONS-06 ozonesondes. Using the Weather Research and Forecasting model with Chemistry (WRF-Chem), we attempt to simulate the ozone enhancement and understand the underlying structure, chemical pathways, and sensitivity to emissions.

Using a modified lightning parameterization based on the Price and Rind scheme, a July-August simulation is performed using WRF-Chem. Validation shows that ash rate is overpredicted by a factor of 10, which subsequently causes an overestimation of O3. Despite the amplified ozone enhancement, boundary layer and stratospheric tracers do not show substantial differences within and outside the anticyclone, contrary to what has been predicted in other studies. On the other hand, lightning tracers, lateral boundary tracers, tracer-tracer correlations, and chemistry pathways can be used to distinguish between the anticyclone and the surrounding area.

Sensitivity and control simulations are also performed to investigate how different emission sources contribute to the ozone enhancement. It is shown that lightning emission enhances NOx superlinearly, which leads to NOx-titration in the upper troposphere. On the other hand, anthropogenic emission is shown to modify the ozone concentration and chemistry profiles via sensitivity to VOC, and biogenic emission affects ozone via sensitivity to NOx. As a result of the changes in ozone mixing ratio profile, convective tendency is also affected, which forms a nonlinear feedback between chemistry and convection in response to perturbation in emissions.

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