Abstract

AbstractPolar stratospheric clouds (PSCs) play important roles in stratospheric ozone depletion during winter and spring at high latitudes (e.g., the Antarctic ozone hole). PSC particles provide sites for heterogeneous reactions that convert stable chlorine reservoir species to radicals that destroy ozone catalytically. PSCs also prolong ozone depletion by delaying chlorine deactivation through the removal of gas‐phase HNO3 and H2O by sedimentation of large nitric acid trihydrate (NAT) and ice particles. Contemporary observations by the spaceborne instruments Michelson Interferometer for Passive Atmospheric Sounding (MIPAS), Microwave Limb Sounder (MLS), and Cloud‐Aerosol Lidar with Orthogonal Polarization (CALIOP) have provided an unprecedented polar vortex‐wide climatological view of PSC occurrence and composition in both hemispheres. These data have spurred advances in our understanding of PSC formation and related dynamical processes, especially the firm evidence of widespread heterogeneous nucleation of both NAT and ice PSC particles, perhaps on nuclei of meteoritic origin. Heterogeneous chlorine activation appears to be well understood. Reaction coefficients on/in liquid droplets have been measured accurately, and while uncertainties remain for reactions on solid NAT and ice particles, they are considered relatively unimportant since under most conditions chlorine activation occurs on/in liquid droplets. There have been notable advances in the ability of chemical transport and chemistry‐climate models to reproduce PSC temporal/spatial distributions and composition observed from space. Continued spaceborne PSC observations will facilitate further improvements in the representation of PSC processes in global models and enable more accurate projections of the evolution of polar ozone and the global ozone layer as climate changes.

Highlights

  • There has been a continuing stream of discoveries about polar stratospheric clouds (PSCs) from the first sightings in the late 19th century to contemporary satellite measurements during the 21st century

  • One possible explanation is that, on average, the size of nitric acid trihydrate (NAT) particles may be larger in the Arctic than in the Antarctic and, less likely to fall into the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) NAT class, which is limited to NAT particles with radii

  • Spaceborne measurements by MIPAS, Microwave Limb Sounder (MLS), and Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) led to the discovery of an Antarctic circumpolar belt of NAT Polar stratospheric clouds (PSCs) triggered by localized cooling events with ice clouds in mountain waves (Höpfner, Larsen et al, 2006; Lambert et al, 2012; Section 4.2)

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Summary

Historical Overview

There has been a continuing stream of discoveries about polar stratospheric clouds (PSCs) from the first sightings in the late 19th century to contemporary satellite measurements during the 21st century The interest in PSCs changed dramatically after the surprising discovery of the Antarctic ozone hole in the 1980s, when it was hypothesized that the clouds might provide the link between anthropogenic chlorine and polar ozone destruction. It was known that they are destroyed by photolysis in the stratosphere, and that the released chlorine could deplete ozone through gas-phase reactions (Molina and Rowland, 1974). The overall depletion was expected to be 5%–10% If this were correct, how could reactions involving chlorine be responsible for the ozone hole, under conditions with little insolation, destroying a major portion of the Antarctic ozone layer?. Polar vortex-wide observations by the contemporary spaceborne instruments Michelson Interferometer for Passive Atmospheric Sounding (MIPAS), Microwave Limb Sounder (MLS), and Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP), a central part of this review paper, have brought about a comprehensive and clearer understanding of PSC spatial and temporal distributions, their conditions of existence, and the processes through which they impact polar ozone

Pre-satellite Era
Early Satellite Measurements
The Years After Discovery of the Ozone Hole
The Golden Era of Satellite PSC Observations
PSC Spatial and Temporal Distributions and Composition
CALIOP
Aura MLS
Ground-Based Lidar Measurements
STS and NAT Particle Detection Sensitivities
CALIOP versus MIPAS
CALIOP Versus Aura MLS
CALIOP Versus Ground-Based Lidar
PSC Characteristics
Overall Seasonal Evolution
PSC Coverage by Composition Class
Geographical and Zonal Mean Distribution
Investigation of Multi-Decadal Trends
Comparison of CALIOP and SAM II PSC Data Records
Comparison of CALIOP and Ground-Based Lidar Records
Formation Pathways and Particle Characteristics
Characteristics of NAT Particles
Evidence for Highly Aspherical β-NAT Particles
Nucleation of NAT Particles
Kinetic Suppression of Homogeneous NAT Nucleation
The Possible Origin of Heterogeneous NAT Nuclei
Formation of Stratospheric Ice Particles
Dynamical Forcing of PSCs
Role of Synoptic Scale Dynamics
Role of Mesoscale Dynamics
Integrated Approach to Synoptic and Mesoscale Dynamical Forcing of PSCs
Representation of Orographic Gravity Waves in Models and Reanalyzes
Seasonal Evolution of Inorganic Chlorine Species
Brief Review of Heterogeneous Reaction Probabilities
Denitrification and Dehydration
Impact of PSCs on Gas Phase Composition
Parameterizations of PSCs in Global Models
Modeling Heterogeneous Chemical Reactions
Size- and Shape-Dependent Particle Sedimentation
Modeling PSCs and Their Impacts
Specific Treatment of PSCs in Different Models
Comparisons of PSC Simulations With Observations
Summary and Outlook
Findings
Data Availability Statement
Full Text
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