Abstract

Abstract. Polar stratospheric clouds (PSCs) contribute to catalytic ozone destruction by providing surfaces for the conversion of inert chlorine species into active forms and by denitrification. The latter describes the removal of HNO3 from the stratosphere by sedimenting PSC particles, which hinders chlorine deactivation by the formation of reservoir species. Therefore, an accurate representation of PSCs in chemistry–climate models (CCMs) is of great importance to correctly simulate polar ozone concentrations. Here, we evaluate PSCs as simulated by the CCM SOCOLv3.1 for the Antarctic winters 2006, 2007 and 2010 by comparison with backscatter measurements by CALIOP on board the CALIPSO satellite. The year 2007 represents a typical Antarctic winter, while 2006 and 2010 are characterized by above- and below-average PSC occurrence. The model considers supercooled ternary solution (STS) droplets, nitric acid trihydrate (NAT) particles, water ice particles and mixtures thereof. PSCs are parameterized in terms of temperature and partial pressures of HNO3 and H2O, assuming equilibrium between the gas and particulate phase. The PSC scheme involves a set of prescribed microphysical parameters, namely ice number density, NAT particle radius and maximum NAT number density. In this study, we test and optimize the parameter settings through several sensitivity simulations. The choice of the value for the ice number density affects simulated optical properties and dehydration, while modifying the NAT parameters impacts stratospheric composition via HNO3 uptake and denitrification. Depending on the NAT parameters, reasonable denitrification can be modeled. However, its impact on ozone loss is minor. The best agreement with the CALIOP optical properties and observed denitrification was for this case study found with the ice number density increased from the hitherto used value of 0.01 to 0.05 cm−3 and the maximum NAT number density from 5×10-4 to 1×10-3 cm−3. The NAT radius was kept at the original value of 5 µm. The new parameterization reflects the higher importance attributed to heterogeneous nucleation of ice and NAT particles following recent new data evaluations of the state-of-the-art CALIOP measurements. A cold temperature bias in the polar lower stratosphere results in an overestimated PSC areal coverage in SOCOLv3.1 by up to 40 %. Offsetting this cold bias by +3 K delays the onset of ozone depletion by about 2 weeks, which improves the agreement with observations. Furthermore, the occurrence of mountain-wave-induced ice, as observed mainly over the Antarctic Peninsula, is continuously underestimated in the model due to the coarse model resolution (T42L39) and the fixed ice number density. Nevertheless, we find overall good temporal and spatial agreement between modeled and observed PSC occurrence and composition. This work confirms previous studies indicating that simplified PSC schemes, which avoid nucleation and growth calculations in sophisticated but time-consuming microphysical process models, may also achieve good approximations of the fundamental properties of PSCs needed in CCMs.

Highlights

  • The occurrence of clouds in the wintertime polar stratosphere has been observed for a long time, their importance for stratospheric ozone depletion was only recognized after the discovery of the Antarctic ozone hole in the mid1980s (Farman et al, 1985)

  • The Antarctic Peninsula, two distinctive regions with very small 1/R532 values are evident. These high backscatter ratios (R532 > 50) are related to high number densities of ice particles, which are caused by rapid cooling rates associated with mountain-wave events. These wave ice clouds are surrounded by more synopticscale Polar stratospheric clouds (PSCs) with lower R532 values, which are classified as ice, supercooled ternary solution (STS) and nitric acid trihydrate (NAT) mixtures

  • We have presented an evaluation of polar stratospheric clouds (PSCs) in the Antarctic stratosphere as simulated by the chemistry–climate model SOCOLv3.1

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Summary

Introduction

The occurrence of clouds in the wintertime polar stratosphere has been observed for a long time, their importance for stratospheric ozone depletion was only recognized after the discovery of the Antarctic ozone hole in the mid1980s (Farman et al, 1985). The detailed PSC formation along different pathways, depending on the presence or absence of heterogeneous nuclei, is usually not taken into account in those models This is no problem under many circumstances, e.g., when chlorine activation is close to saturation in the middle of an Antarctic winter, but accurate knowledge of the heterogeneous reaction and denitrification rates is essential for a quantitative description of polar ozone chemistry under transitional conditions, as they occur at winter onset, in late winter and early spring, or at the far edge of the vortex. We compare a simple equilibrium scheme of STS, NAT, ice and mixtures thereof with state-of-theart PSC satellite data, aiming to optimize the scheme for economic and efficient use in a chemistry–climate model (CCM) To this end, we evaluate the representation of PSCs in the CCM SOCOLv3.1 for the Antarctic winters 2006, 2007 and 2010.

Model description and observational data
CALIPSO PSC observations
Model–measurement comparison
MLS observations
Results and discussion
Comparison along an orbit
Spatial distribution
PSC areal coverage
Sensitivity to microphysical parameters
Discussion and conclusions
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