Date of Award

Spring 2009

Project Type

Dissertation

Program or Major

Earth and Environmental Sciences

Degree Name

Doctor of Philosophy

First Advisor

Huiting Mao

Abstract

This dissertation focused on the impact of circulation, a key climate variable, on air quality from regional to global scale. The relationships between circulation and tropospheric ozone (O3) levels were investigated for the surface over the northeastern U.S. as well as for the spring-, winter- and summertime North American export and trans-Atlantic Transport. The latter studies utilized the Tropospheric Emission Spectrometer (TES) retrievals of O3 and carbon monoxide (CO) to explore the three-dimensional structure of continental outflow and to identify anthropogenic influence on the free troposphere over the remote oceanic region. The key findings are summarized as follows. First, the most common among the top five circulation patterns across the northeastern U.S. for summers 2000-2004, identified with a correlation-based synoptic categorization technique, was associated with stagnant warm conditions that were intimately associated with occurrence of high O3. O 3 varied on an interannual timescale from a mean daily maximum value of 64 ppbv in 2002 to 52 ppbv in 2004. The sea level pressure (SLP) system intensity and frequency of each map type accounted for 46% of the interannual variability. The remainder was possibly due to non-linear relationships between climate and biogenic emissions and decreasing power plant emissions over the analysis period. Second, during spring continental export was evident from enhanced O3 (>55 ppbv) and CO (>115 ppbv) at the 681 hPa retrieval level suggesting anthropogenic influence. The export was found to be facilitated by both the primary and secondary branches of the warm conveyor belt (WCB) of cyclones which lofted pollutants from the continental boundary layer to the free troposphere enabling fast long distance transport with subsequent global impact. Ample evidence suggested stratospheric intrusions associated with cyclonic circulations particularly to the north of 45°N. Third, during winter the O3 levels at 681 hPa were uniformly low (∼45 ppbv) and the continental export was only evident in enhanced CO. Export to the free troposphere was mainly via the WCB and shallow convection behind cold fronts resulting from cold air flowing over warmer ocean waters. In summer O3 levels were highly variable and the main export band was shifted northward around the Bermuda High, except during the passage of weak cyclones and cold fronts when export was shifted further south.

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