NOy partitioning and budget and its correlation with N2O in the Arctic vortex and in summer midlatitudes in 1997

Abstract

Vertical profiles of the most important species of nocturnal total reactive nitrogen (NOy = NO2 + HNO3 + ClONO2 + 2 N2O5 + HO2NO2) together with its source gas N2O were retrieved from infrared limb emission spectra measured by the Michelson Interferometer for Passive Atmospheric Sounding, Balloon‐borne version (MIPAS‐B) instrument inside the late winter arctic vortex from Kiruna (Sweden, 68°N) on 24 March 1997 and in summer midlatitudes from Gap (France, 44°N) on 2 July 1997. The measured data were compared to calculations performed with the three‐dimensional chemistry transport model (CTM) Karlsruhe Simulation model of the Middle Atmosphere (KASIMA). The results show that in the late winter arctic vortex most of the available nitrogen and chlorine is in the form of HNO3 and ClONO2, respectively. An anomalous N2O‐NOy correlation observed in March 1997 appears to be caused to a large extent by quasi‐horizontal mixing of air masses across the vortex edge. However, near 20 km some denitrification of ∼1.5 to 2 ppbv NOy could be observed. The N2O profile measured in July 1997 indicates remnants of polar vortex air and is not reproduced by the CTM at the same location. However, the profile shapes of the individual compounds of the NOy family as well as the NOx/NOy ratio are reproduced fairly well by the model.