ALBERT

Description: During several balloon flights inside the Arctic polar vortex in early 2003, unusual trace gas distributions were observed, which indicate a strong influence of mesospheric air in the stratosphere. The tuneable diode laser (TDL) instrument SPIRALE (Spectroscopie InFrarouge par Absorption de Lasers Embarqués) measured unusually high CO values (up to 600 ppb) on 27 January at about 30 km altitude. The cryosampler BONBON sampled air masses with very high molecular Hydrogen, extremely low SF6 and enhanced CO values on 6 March at about 25 km altitude. Finally, the MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) Fourier Transform Infra-Red (FTIR) spectrometer showed NOy values which are significantly higher than NOy* (the NOy derived from a correlation between N2O and NOy under undisturbed conditions), on 21 and 22 March in a layer centred at 22 km altitude. Thus, the mesospheric air seems to have been present in a layer descending from about 30 km in late January to 25 km altitude in early March and about 22 km altitude on 20 March. We present corroborating evidence from a model study using the KASIMA (KArlsruhe Simulation model of the Middle Atmosphere) model that also shows a layer of mesospheric air, which descended into the stratosphere in November and early December 2002, before the minor warming which occurred in late December 2002 lead to a descent of upper stratospheric air, cutting of a layer in which mesospheric air is present. This layer then descended inside the vortex over the course of the winter. The same feature is found in trajectory calculations, based on a large number of trajectories started in the vicinity of the observations on 6 March. Based on the difference between the mean age derived from SF6 (which has an irreversible mesospheric loss) and from CO2 (whose mesospheric loss is much smaller and reversible) we estimate that the fraction of mesospheric air in the layer observed on 6 March, must have been somewhere between 35% and 100%.

Description: Simulations of Arctic denitrification using a 3-D chemistry-microphysics transport model are compared with observations for the winters 1994/1995, 1996/1997 and 1999/2000. The model of Denitrification by Lagrangian Particle Sedimentation (DLAPSE) couples the full chemical scheme of the 3-D chemical transport model, SLIMCAT, with a nitric acid trihydrate (NAT) growth and sedimentation scheme. We use observations from the Microwave Limb Sounder (MLS) and Improved Limb Atmospheric Sounder (ILAS) satellite instruments, the balloon-borne Michelsen Interferometer for Passive Atmospheric Sounding (MIPAS-B), and the in situ NOy instrument on-board the ER-2. As well as directly comparing model results with observations, we also assess the extent to which these observations are able to validate the modelling approach taken. For instance, in 1999/2000 the model captures the temporal development of denitrification observed by the ER-2 from late January into March. However, in this winter the vortex was already highly denitrified by late January so the observations do not provide a strong constraint on the modelled rate of denitrification. The model also reproduces the MLS observations of denitrification in early February 2000. In 1996/1997 the model captures the timing and magnitude of denitrification as observed by ILAS, although the lack of observations north of ~67° N make it difficult to constrain the actual timing of onset. The comparison for this winter does not support previous conclusions that denitrification must be caused by an ice-mediated process. In 1994/1995 the model notably underestimates the magnitude of denitrification observed during a single balloon flight of the MIPAS-B instrument. Agreement between model and MLS HNO3 at 68 hPa in mid-February 1995 was significantly better. Sensitivity tests show that a 1.5 K overall decrease in vortex temperatures or a factor 4 increase in assumed NAT nucleation rates produce the best statistical fit to MLS observations. Both adjustments would be required to bring the model into agreement with the MIPAS-B observations. The agreement between the model and observations suggests that a NAT-only denitrification scheme (without ice), which was discounted by previous studies, must now be considered as one mechanism for the observed Arctic denitrification. The timing of onset and the rate of denitrification remain poorly constrained by the available observations.