Climate Chemistry Coupling: Ozone Loss Linked to the Unique Dynamical Structure of the Summertime Stratosphere Over the U.S. Using In Situ Aircraft, Satellite and NEXRAD Radar Observations

Abstract:

A remarkable combination of meteorological and catalytic chemical factors place the summertime lower stratosphere over the U.S. in a unique position at the intersection of climate forcing and potential ozone loss in the stratosphere. The factors that conspire to establish this circumstance engages four independent considerations. First is the occurrence of severe storms in the U.S. Mid-West caused by the intersection of moist airflow from the Gulf of Mexico with airflow from higher latitudes in spring and summer. These storms are characterized by a combination of tornadoes, hail, heavy precipitation and high winds, the frequency and intensity of which are increasing with increased forcing of the climate system by the addition of CO₂, CH₄, N₂O CFCs, and other infrared active species to the atmosphere associated with human activity. Second is the recognition that these severe storms are capable of injecting water vapor deep into the stratosphere over the U.S., with injection depths reaching the altitude of increasing inorganic halogen species formed by the photolytic breakdown of organic chorine and bromine transported into the stratosphere. Third is the recognition that the catalytic conversion of inorganic halogen species to radicals, specifically ClO and BrO, that are the rate limiting catalytic species that destroy ozone, occurs on ubiquitous sulfate-water aerosols wherever and whenever the temperature-water vapor conditions are met. These conditions are met in the Antarctic and Arctic winter vortices by virtue of temperatures below 200K at 5 ppmv water vapor, and in the summertime lower stratosphere over the U.S. by virtue of temperatures between 200 and 205K in combination with convectively injected water vapor concentrations in the range of 8 ppmv or greater. Fourth, is the recognition that the flow pattern of the lower stratosphere over the U.S. in summer is repeatedly under the control of the North American monsoon that forms an anti-cyclonic (clockwise) gyre that captures the combination of chemical species within it, retaining that chemical mix for periods up to three weeks during the months of July and August. It is within this gyre over the U.S. that the catalytic reactions can occur potentially reducing the column concentration of ozone in summer.