Mp. Chipperfield et al., ANALYSIS OF UARS DATA IN THE SOUTHERN POLAR VORTEX IN SEPTEMBER 1992 USING A CHEMICAL-TRANSPORT MODEL, JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 101(D13), 1996, pp. 18861-18881
We have used a new, isentropic-coordinate three-dimensional chemical t
ransport model to investigate the decay of ClO and evolution of other
species in the Antarctic polar vortex during September 1992. The model
simulations cover the same southern hemisphere period studied in a co
mpanion data paper by Santee et al. [this issue]. The model is initial
ized using the available data from the Microwave Limb Sounder (MLS) an
d Cryogenic Limb Array Etalon Spectrometer (CLAES) on the Upper Atmosp
here Research Satellite (UARS). During the model initialization chemic
al inconsistencies in the UARS data became evident. Fields of odd nitr
ogen (NOy) derived from CLAES N2O underestimated the sum of the direct
observations of the major NOy species. Results from the model integra
tions at 465 K and 585 K are sampled in the same way as the various UA
RS instruments and compared to the observations both directly and by c
onsidering average quantities in the inner and edge vortex regions. Sa
mpling the observed species ill the same way as the UARS instruments i
s important in removing any spurious trends due, for example, to chang
ing solar zenith angle. While the model can reproduce the magnitude of
the MLS ClO observations at 585 K, this is not possible at 465 K. The
model partitions too much ClO into Cl2O2 to reproduce the observed Cl
O which is around 2.0 parts per billion by volume (ppbv) averaged with
in the polar vortex. The model also underestimates CLAES ClONO2 in the
inner vortex at 465 K due to heterogeneous processing. The observatio
ns require that effectively all of the inorganic chlorine is in the fo
rm of ClO and C1ONO2 in the inner vortex at this altitude. In the basi
c model run, the decay of ClO produces ClONO2 which is not observed by
CLAES. Our results indicate the potential importance of the speculati
ve reaction between OH and ClO producing HCl for the recovery of HCl i
n the Antarctic spring. By including this reaction, the decay of model
ClO into HCl is enhanced, yielding better agreement with HCl data fro
m the Halogen Occultation Experiment (HALOE) data. Similar results can
also be obtained by including the reaction between HO2 and ClO to pro
duce HCl with a 3% channel. The model generally reproduces the observe
d O-3 destruction during September. The most significant discrepancy f
or O-3 is in the inner vortex at 465 K where the model underestimates
the observed O-3 loss rate, especially when the effects of vertical mo
tion are included.