Gwenael Berthet

Polar vortex evolution during the 2002 Antarctic major warming as observed by the Odin satellite

In September 2002 the Antarctic polar vortex split in two under the influence of a sudden warming. During this event, the Odin satellite was able to measure both ozone (O3) and chlorine monoxide (ClO), a key constituent responsible for the so-called “ozone hole”, together with nitrous oxide (N2O), a dynamical tracer, and nitric acid (HNO3) and nitrogen dioxide (NO2), tracers of denitrification. The submillimeter radiometer (SMR) microwave instrument and the Optical Spectrograph and Infrared Imager System (OSIRIS) UV-visible light spectrometer (VIS) and IR instrument on board Odin have sounded the polar vortex during three different periods: before (19–20 September), during (24–25 September), and after (1–2 and 4–5 October) the vortex split. Odin observations coupled with the Reactive Processes Ruling the Ozone Budget in the Stratosphere (REPROBUS) chemical transport model at and above 500 K isentropic surfaces (heights above 18 km) reveal that on 19–20 September the Antarctic vortex was dynamically stable and chemically nominal: denitrified, with a nearly complete chlorine activation, and a 70% O3 loss at 500 K. On 25–26 September the unusual morphology of the vortex is monitored by the N2O observations. The measured ClO decay is consistent with other observations performed in 2002 and in the past. The vortex split episode is followed by a nearly complete deactivation of the ClO radicals on 1–2 October, leading to the end of the chemical O3 loss, while HNO3 and NO2 fields start increasing. This acceleration of the chlorine deactivation results from the warming of the Antarctic vortex in 2002, putting an early end to the polar stratospheric cloud season. The model simulation suggests that the vortex elongation toward regions of strong solar irradiance also favored the rapid reformation of ClONO2. The observed dynamical and chemical evolution of the 2002 polar vortex is qualitatively well reproduced by REPROBUS. Quantitative differences are mainly attributable to the too weak amounts of HNO3 in the model, which do not produce enough NO2 in presence of sunlight to deactivate chlorine as fast as observed by Odin.

Nighttime chlorine monoxide observations by the Odin satellite and implications for the ClO/Cl2O2 equilibrium

We use measurements of chlorine monoxide (ClO) by the SMR instrument onboard the Odin satellite to study the nighttime thermal equilibrium between ClO and its dimer Cl2O2. Observations performed in the polar vortex during the 2002-2003 Arctic winter showed enhanced amounts of nighttime ClO over a wide range of stratospheric temperatures (185 < T < 225 K). Odin/SMR measurements are here compared to three-dimensional model calculations using various published estimations of the K-eq equilibrium constant between ClO and Cl2O2. Our results show that the value of K-eq currently recommended by JPL (Sander et al., 2003) leads to a large underestimation of the observed nighttime ClO amounts, and that a realistic estimation of K-eq must lie between the values determined by Cox and Hayman (1988) and Von Hobe et al. (2005).

Intercomparisons of trace gases profiles from the Odin/SMR and Aura/MLS limb sounders

This paper presents the intercomparison of O(3), HNO(3), ClO, N(2)O and CO profiles measured by the two spaceborne microwave instruments MLS ( Microwave Limb Sounder) and SMR ( Submillimetre Radiometer) on board the Aura and Odin satellites, respectively. We compared version 1.5 level 2 data from MLS with level 2 data produced by the French data processor version 222 and 225 and by the Swedish data processor version 2.0 for several days in September 2004 and in March 2005. For the five gases studied, an overall good agreement is found between both instruments. Most of the observed discrepancies between SMR and MLS are consistent with results from other intercomparison studies involving MLS or SMR. O(3) profiles retrieved from the SMR 501.8 GHz band are noisier than MLS profiles but mean biases between both instruments do not exceed 10%. SMR HNO(3) profiles are biased low relative to MLSs by similar to 30% above the profile peak. In the lower stratosphere, MLS ClO profiles are biased low by up to 0.3 ppbv relative to coincident SMR profiles, except in the Southern Hemisphere polar vortex in the presence of chlorine activation. N(2)O profiles from both instruments are in very good agreement with mean biases not exceeding 15%. Finally, the intercomparison between SMR and MLS CO profiles has shown a good agreement from the middle stratosphere to the middle mesosphere in spite of strong oscillations in the MLS profiles. In the upper mesosphere, MLS CO concentrations are biased high relative to SMR while negative values in the MLS retrievals are responsible for a negative bias in the tropics around 30 hPa.

A stratospheric NO2 climatology from Odin/OSIRIS limb-scatter measurements

A climatology of stratospheric nitrogen dioxide (NO2), in terms of mean and standard deviation, as a function of latitude (5° bins); altitude (10–46 km in 2 km bins); local solar time (24 h); and month is constructed based on the Odin/OSIRIS limb-scattering data from 2002–2005. The measured profiles, given at specific local solar times, are scaled to all 24 h using a photochemical box model. The Odin orbit gives near global coverage around the equinoxes and hemispheric coverage elsewhere, due to lack of sunlight. The mean NO2 field at a specific local solar time involves high concentrations in the polar summer, peaking at around 25 km, with a negative equatorward gradient. Distinct high levels between 40–50° latitude at 30 km in the winter/spring hemisphere are also found, associated with the so-called {Noxon-cliff}. The diurnal cycle reveals the lowest NO2 concentrations just after sunrise and steep gradients at twilight. The 1σ standard deviation is generally quite low, around 20%, except for winter and spring high latitudes, where values are well above 50% and stretch through the entire stratosphere, a phenomenon probably related to the polar vortex. It is also found that NO2 concentrations are log-normally distributed. Comparisons to a climatology based on data from a (REPROBUS) chemical transport model for the same time period reveal relative differences below 20% in general, which is comparable to the estimated OSIRIS systematic uncertainty. Clear exceptions are the polar regions in winter/spring throughout the atmosphere and equatorial regions below 25 km, where OSIRIS is relatively higher by 40% and more. These discrepancies are most likely attributable to limitations of the model, but this has to be investigated further.

Ultraviolet–visible bulk optical properties of randomly distributed soot

The presence of soot in the lower stratosphere was recently established by in situ measurements. To isolate their contribution to optical measurements from that of background aerosol, the soots bulk optical properties must be determined. Laboratory measurements of extinction and polarization of randomly distributed soot were conducted. For all soot, measurements show a slight reddening extinction between 400 and 700 nm and exhibit a maximum of 100% polarization at a scattering angle of 75 +/- 5 degrees. Such results cannot be reproduced by use of Mie theory assumptions. The different optical properties of soot and background stratospheric aerosol could allow isolation of soot in future analyses of stratospheric measurements.