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Massive Australian wildfires lofted smoke directly into the stratosphere in the austral summer of 2019/20. The smoke led to increases in optical extinction throughout the midlatitudes of the southern hemisphere that rivalled substantial volcanic perturbations. Previous studies have assumed that the smoke became coated with sulfuric acid and water and would deplete the ozone layer through heterogeneous chemistry on those surfaces, as is routinely observed following volcanic enhancements of the stratospheric sulfate layer. Here, observations of extinction and reactive nitrogen species from multiple independent satellites that sampled the smoke region are compared to one another and to model calculations. The data display a strong decrease in reactive nitrogen concentrations with increased aerosol extinction in the stratosphere, which is a known fingerprint for key heterogeneous chemistry on sulfate/H₂O particles (specifically the hydrolysis of N₂O₅ to form HNO₃). This chemical shift affects not only reactive nitrogen but also chlorine and reactive hydrogen species and is expected to cause midlatitude ozone layer depletion. Comparison of the model ozone to observations suggests that N₂O₅ hydrolysis contributed to reduced ozone, but additional chemical and/or dynamical processes are also important. These findings suggest that if wildfire smoke injection into the stratosphere increases sufficiently in frequency and magnitude as the world warms due to climate change, ozone recovery under the Montreal Protocol could be impeded, at least sporadically. Modeled austral midlatitude total ozone loss was about 1% in March 2020, which is significant compared to expected ozone recovery of about 1% per decade.

Tropospheric ozone (O 3 ) is a key component of air pollution and an important anthropogenic greenhouse gas 1 . During the twentieth century, the proliferation of the internal combustion engine, rapid industrialization and land-use change led to a global-scale increase in O 3 concentrations 2 , 3 ; however, the magnitude of this increase is uncertain. Atmospheric chemistry models typically predict 4 – 7 an increase in the tropospheric O 3 burden of between 25 and 50 per cent since 1900, whereas direct measurements made in the late nineteenth century indicate that surface O 3 mixing ratios increased by up to 300 per cent 8 – 10 over that time period. However, the accuracy and diagnostic power of these measurements remains controversial 2 . Here we use a record of the clumped-isotope composition of molecular oxygen ( 18 O 18 O in O 2 ) trapped in polar firn and ice from 1590 to 2016 ad , as well as atmospheric chemistry model simulations, to constrain changes in tropospheric O 3 concentrations. We find that during the second half of the twentieth century, the proportion of 18 O 18 O in O 2 decreased by 0.03 ± 0.02 parts per thousand (95 per cent confidence interval) below its 1590–1958 ad mean, which implies that tropospheric O 3 increased by less than 40 per cent during that time. These results corroborate model predictions of global-scale increases in surface pollution and vegetative stress caused by increasing anthropogenic emissions of O 3 precursors 4 , 5 , 11 . We also estimate that the radiative forcing of tropospheric O 3 since 1850 ad is probably less than +0.4 watts per square metre, consistent with results from recent climate modelling studies 12 . Isotope data from polar firn and ice are used to constrain the increase in tropospheric ozone between 1850 and 2005 ad .

The interaction of stratospheric chemistry with a changing climate from an abrupt CO2 quadrupling is assessed using the coupled atmosphere–ocean Goddard Earth Observing System Chemistry-Climate Model (GEOSCCM). Two abrupt 4 × CO2 experiments were performed, one with interactive stratospheric chemistry and the other with a prescribed stratospheric chemistry that does not simulate stratospheric ozone response to 4 × CO2. The interactive and prescribed chemistry experiments simulate similar global mean surface temperature change. Nevertheless, interactive chemistry is critical to capture the Southern Hemisphere tropospheric midlatitude jet response to 4 × CO2. When stratospheric ozone response to 4 × CO2 is neglected, GEOSCCM overestimates Southern Hemisphere tropospheric circulation change. This stratospheric chemistry-induced climate impact has large seasonal variability. During the austral spring season September–October–November (SON), prescribed chemistry yields a stronger poleward shift and intensification of the Southern Hemisphere midlatitude tropospheric jet, surface wind stress, and the Southern Ocean meridional overturning circulation than occurs with interactive chemistry. In other seasons interactive and prescribed chemistry have similar effects on the Southern Hemisphere circulation. The seasonality of stratospheric chemistry-induced climate impact is related to the seasonality of Antarctic lower stratospheric ozone response to 4 × CO2. In contrast to this stratospheric ozone response to 4 × CO2, stratospheric ozone recovery from decline of the ozone depleting substances has its largest impact on the Southern Hemisphere tropospheric circulation in austral summer (December–January–February), but no effects in SON. It is found that the different seasonality for these two stratospheric ozone layer change scenarios is related to the different seasonality of tropopause meridional temperature gradient response.

Nitrous oxide (N₂O) is the largest known remaining anthropogenic threat to the stratospheric ozone layer. However, it is currently only regulated under the 1997 Kyoto Protocol because of its simultaneous ability to warm the climate. The threat N₂O poses to the stratospheric ozone layer, coupled with the uncertain future of the international climate regime, motivates our exploration of issues that could be relevant to the Parties to the ozone regime (the 1985 Vienna Convention and its 1987 Montreal Protocol) should they decide to take measures to manage N₂O in the future. There are clear legal avenues to regulate N₂O under the ozone regime as well as several ways to share authority with the existing and future international climate treaties. N₂O mitigation strategies exist to address the most significant anthropogenic sources, including agriculture, where behavioral practices and new technologies could contribute significantly to reducing emissions, Existing policies managing N₂O and other forms of reactive nitrogen could be harnessed and built on by the ozone regime to implement N₂O controls. There are several challenges and potential cobenefits to N₂O control which we discuss here: food security, equity, and implications of the nitrogen cascade. The possible inclusion of N₂O in the ozone regime need not be viewed as a sign of failure of the United Nations Framework Convention on Climate Change to adequately deal with climate change. Rather, it could represent an additional valuable tool in sustainable development diplomacy.

We here reflect on two important articles on stratospheric ozone depletion written by P. J. Crutzen (1974) and P. J. Crutzen and D. H. Ehhalt (1977) in the early 1970s. These articles provide a clear description of the stratosphere and the most important chemical reactions involved in stratospheric ozone depletion. They present modeling results and provide recommendations for future research on stratospheric ozone depletion caused by chloro-fluoro-carbons, supersonic transport, nitrous oxide, and nuclear explosions. These two articles represent the beginning of a scientific era, which led to discovery of the Antarctic ozone hole and political action in the form of the Montreal Protocol and its amendments.

The absolute value of total solar irradiance is not known to better than ca.0.3% but measurements from satellite instruments over the past two solar cycles have shown that it varies by ca.0.1% on this time-scale. Over longer periods its value has been reconstructed using proxy measures of solar activity, and these suggest that during the Maunder minimum in solar activity of the late 17th century it was 3−4 W m−2 lower than at present. Observational data suggest that the Sun has influenced temperatures on decadal, centennial and millennial time-scales, but radiative forcing considerations and the results of energy-balance models and general circulation models suggest that the warming during the latter part of the 20th century cannot be ascribed entirely to solar effects. However, chemical and dynamical processes in the middle atmosphere may act to amplify the solar impact. An analysis of zonal mean temperature data shows that solar effects may be differentiated from those associated with other factors such as volcanic eruptions and the El Niño Southern Oscillation.

Surface ultraviolet (UV) radiation plays an important role in human health. Increased exposure to UV radiation increases the risk of skin cancer. In Australia, public campaigns to prevent skin cancer include the promotion of daily UV forecasts. If all other atmospheric factors are equal, stratospheric ozone decreases result in UV increases. Given that Australia still has the highest skin cancer rates in the world, it is important to monitor Australia’s stratospheric ozone and UV radiation levels over time because of the effects cumulative exposure can have on humans. In this paper, two long-term ozone datasets derived from surface and satellite measurements, a radiation code and atmospheric meteorological fields are used to calculate clear-sky UV radiation over a 50-year period (1959–2009) for Australia. The deviations from 1970–1980 levels show that clear-sky UV is on the rise. After the 1990s, an overall annual increase from 2 to 6% above the 1970–1980 levels was observed at all latitudes. Examining the summer and winter deviations from 1970–1980 showed that the winter signal dominated the annual changes, with winter increases almost twice those in summer. With ozone levels not expected to recover to pre-depletion levels until the middle of this century, UV levels are expected to continue to rise. Combined with Australians favoring an outdoor life-style, when temperatures are warmer, under high levels of UV, the associated risk of skin cancer will increase.

Ozone profile trends over the period 2000 to 2016 from several merged satellite ozone data sets and from ground-based data measured by four techniques at stations of the Network for the Detection of Atmospheric Composition Change indicate significant ozone increases in the upper stratosphere, between 35 and 48 km altitude (5 and 1 hPa). Near 2 hPa (42 km), ozone has been increasing by about 1.5 % per decade in the tropics (20° S to 20° N), and by 2 to 2.5 % per decade in the 35 to 60° latitude bands of both hemispheres. At levels below 35 km (5 hPa), 2000 to 2016 ozone trends are smaller and not statistically significant. The observed trend profiles are consistent with expectations from chemistry climate model simulations. This study confirms positive trends of upper stratospheric ozone already reported, e.g., in the WMO/UNEP Ozone Assessment 2014 or by Harris et al. (2015). Compared to those studies, three to four additional years of observations, updated and improved data sets with reduced drift, and the fact that nearly all individual data sets indicate ozone increase in the upper stratosphere, all give enhanced confidence. Uncertainties have been reduced, for example for the trend near 2 hPa in the 35 to 60° latitude bands from about ±5 % (2σ) in Harris et al. (2015) to less than ±2 % (2σ). Nevertheless, a thorough analysis of possible drifts and differences between various data sources is still required, as is a detailed attribution of the observed increases to declining ozone-depleting substances and to stratospheric cooling. Ongoing quality observations from multiple independent platforms are key for verifying that recovery of the ozone layer continues as expected.

In this review, instead of summarizing all the advances and progress achieved in stratospheric research, the main advances and new developments in stratosphere-troposphere coupling and stratospheric chemistry-climate interactions are summarized, and some outstanding issues and grand challenges are discussed. A consensus has been reached that the stratospheric state is an important source of improving the predictability of the troposphere on sub-seasonal to seasonal (S2S) time scales and beyond. However, applying stratospheric signals in operational S2S forecast models remains a challenge because of model deficiencies and the complexities of the underlying mechanisms of stratosphere-troposphere coupling. Stratospheric chemistry, which controls the magnitude and distribution of many important climate-forcing agents, plays a critical role in global climate change. Convincing evidence has been found that stratospheric ozone depletion and recovery have caused significant tropospheric climate changes, and more recent studies have revealed that stratospheric ozone variations can even exert an impact on SSTs and sea ice. The climatic impacts of stratospheric aerosols and water vapor are also important. Although their quantitative contributions to radiative forcing have been reasonably well quantified, there still exist large uncertainties in their long-term impacts on climate. The advances and new levels of understanding presented in this review suggest that whole-atmosphere interactions need to be considered in future for a better and more thorough understanding of stratosphere-troposphere coupling and its role in climate change.

Compared to stratospheric SO2 injection for climate intervention, alumina particle injection could reduce stratospheric warming and associated adverse impacts. However, heterogeneous chemistry on alumina particles, especially chlorine activation via ClONO2+HCl→surfCl2+HNO3${\\text{ClONO}}_{2}+\\text{HCl}\\stackrel{\\text{surf}}{\\to }{\\text{Cl}}_{2}+{\\text{HNO}}_{3}$ , is poorly constrained under stratospheric conditions, such as low temperature and humidity. This study quantifies the uncertainty in modeling the ozone response to alumina injection. We show that extrapolating the limited experimental data for ClONO2 + HCl to stratospheric conditions leads to uncertainties in heterogeneous reaction rates of almost two orders of magnitude. Implementation of injection of 5 Mt/yr of particles with 240 nm radius in an aerosol‐chemistry‐climate model shows that resulting global total ozone depletions range between negligible and as large as 9%, that is more than twice the loss caused by chlorofluorocarbons, depending on assumptions on the degree of dissociation and interaction of the acids HCl, HNO3, and H2SO4 on the alumina surface. Plain Language Summary Global warming caused by increasing greenhouse gases could be temporarily reduced by introducing aerosol particles into the stratosphere. The most frequently studied approach to climate intervention uses H2SO4‐H2O aerosols, which, however, could result in undesirably strong warming of the stratosphere and significant ozone depletion. This might be improved by injecting solid particles, for example, made of aluminum oxide. However, here we show that the extremely limited availability of experimental studies on heterogeneous chemistry on alumina under the influence of stratospheric concentrations of HCl, HNO3, H2SO4, and H2O leads to large uncertainties in the impact of alumina injection on stratospheric ozone. In order to quantify these uncertainties, we integrated the currently available knowledge about the most important heterogeneous reaction ClONO2+HCl→surfCl2+HNO3${\\text{ClONO}}_{2}+\\text{HCl}\\stackrel{\\text{surf}}{\\to }{\\text{Cl}}_{2}+{\\text{HNO}}_{3}$into an aerosol‐chemistry‐climate model. We conclude that the uncertainty in the resulting heterogeneous reaction rate is more than two orders of magnitude depending on the partitioning of HCl, H2SO4, and HNO3 on the alumina surface. This could lead to global ozone column depletion ranging between almost negligible and up to 9%, which would be more than twice as much as the ozone loss caused by chlorofluorocarbons in the late 1990s. Key Points Heterogeneous chemistry on solid alumina particles is highly uncertain and depends strongly on the partitioning of acids onto the surface The reaction rate of ClONO2 with HCl on alumina particles is uncertain by up to two orders of magnitude under stratospheric conditions Injection of 5 Mt/yr of alumina particles could double global ozone reductions compared to chlorofluorocarbons in the late 1990s