Redistribution of nitric acid in the Arctic lower stratosphere during the winter of 1996–1997

Vertical profiles of HNO 3 , N 2 O, O 3 , and the aerosol extinction coefficient at 780 nm were observed by the Improved Limb Atmospheric Spectrometer (ILAS) on board the Advanced Earth Observing Satellite (ADEOS) during the Arctic winter of 1996-1997. Irreversible redistribution of HNO 3 is evaluated using HNO 3 -N 2 O and HNO 3 -O 3 correlations. Denitrification and nitrification started to be observed just after the Arctic vortex cooled to below the ice frost point (T ICE ) on February 10. Trajectory analyses show that denitrification occurred only in air masses, which were once cooled to near T ICE and were kept at temperatures below the nitric acid trihydrate saturation threshold continuously for more than 4 days. Such a temperature history provides the necessary conditions for nucleation and growth of particles causing denitrification. The average extent of denitrification at 19 km reached 43% at the center of the vortex, suggesting that stratospheric ozone could be affected by denitrification deep inside the vortex. Denitrification (>2 ppbv) and nitrification (> 1 ppbv) covered 40±10% and 35±10% of the vortex area, respectively. Redistributed numbers of HNO 3 molecules at each altitude were calculated by integrating the area-weighted changes in the HNO 3 concentration. The decreases in total HNO 3 concentration at 17-21 km in late February and early March agreed with the increases at 12-15 km to within 25%, confirming conservation of HNO 3 during sedimentation and evaporation of HNO 3 -containing polar stratospheric cloud particles.

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