Observations of large reductions in the NO/NO_y ratio near the mid-latitude tropopause and the role of heterogeneous chemistry

Abstract

During the 1993 NASA Stratospheric Photochemistry, Aerosols and Dynamics Expedition (SPADE), anomalously low nitric oxide (NO) was found in a distinct sunlit layer located above the mid-latitude tropopause. The presence of a significant amount of reactive nitrogen (NO_y) in the layer implies the systematic removal of NO, which is without precedent in stratospheric in situ observations. Large increases in measured chlorine monoxide (ClO) and the hydroperoxyl radical (HO_2) also were observed in the layer. Heterogeneous reaction rate constants of chlorine nitrate (ClONO_2) with hydrogen chloride (HCl) and H_2O to form nitric acid (HNO_3) on sulfate aerosol are enhanced in the NO removal layer by local increases in H_2O and aerosol surface area. The associated conversion of NO_x (= NO + NO_2) to HNO_3 is the most likely cause of the observed low NO and NO_x/NO_y values and high ClO values.

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