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In contrast to the general stratospheric ozone recovery following international agreements, recent observations show an ongoing net ozone depletion in the tropical lower stratosphere (LS). This depletion is thought to be driven by dynamical transport accelerated by global warming, while chemical processes have been considered to be unimportant. Here we use a chemistry–climate model to demonstrate that halogenated ozone-depleting very short-lived substances (VSLS) chemistry may account for around a quarter of the observed tropical LS negative ozone trend in 1998–2018. VSLS sources include both natural and anthropogenic emissions. Future projections show the persistence of the currently unaccounted for contribution of VSLS to ozone loss throughout the twenty-first century in the tropical LS, the only region of the global stratosphere not projecting an ozone recovery by 2100. Our results show the need for mitigation strategies of anthropogenic VSLS emissions to preserve the present and future ozone layer in low latitudes.

In contrast to the general stratospheric ozone recovery following international agreements, recent observations show an ongoing net ozone depletion in the tropical lower stratosphere (LS). This depletion is thought to be driven by dynamical transport accelerated by global warming, while chemical processes have been considered to be unimportant. Here we use a chemistry–climate model to demonstrate that halogenated ozone-depleting very short-lived substances (VSLS) chemistry may account for around a quarter of the observed tropical LS negative ozone trend in 1998–2018. VSLS sources include both natural and anthropogenic emissions. Future projections show the persistence of the currently unaccounted for contribution of VSLS to ozone loss throughout the twenty-first century in the tropical LS, the only region of the global stratosphere not projecting an ozone recovery by 2100. Our results show the need for mitigation strategies of anthropogenic VSLS emissions to preserve the present and future ozone layer in low latitudes.

Air pollution is a major environmental threat to human health. Pollutants can reach extreme levels in the lower atmosphere when weather conditions permit. As pollutant concentrations depend on scales and processes that are not fully represented in current global circulation models (GCMs), and it is often too computationally expensive to run models with atmospheric chemistry and aerosol processes, air stagnation is often used as a proxy for pollution events with particular success in Europe. However, the variables required to identify air stagnation can have biases in GCM output, which adds uncertainty to projected trends in air stagnation. Here, the representation of air stagnation in GCMs is assessed for Europe in the historical period and in end-of-century projections based on a high-emission scenario using three methods for identifying air stagnation. The monthly frequency of stagnation during summer and autumn is projected to increase with climate change when stagnation is identified by a well-established index. However, this increase is not present when air-stagnation frequency is estimated using a statistical model based on the synoptic- to large-scale atmospheric circulation. This implies that the projected increases in air stagnation are not driven by an increase in frequency or severity of large-scale circulation events that are conducive to stagnation. Indeed, projected changes to the atmospheric circulation in GCMs, in particular a reduction in atmospheric block frequency, would suggest a reduction in future air stagnation. Additional analyses indicate that the projected increases in stagnation frequency follow the trend toward more frequent dry days, which is apparently unrelated to the large-scale drivers of air stagnation.

The Brewer-Dobson Circulation (BDC) determines the distribution of long-lived tracers in the stratosphere; therefore, their changes can be used to diagnose changes in the BDC. We evaluate decadal (2005–2018) trends of nitrous oxide (N2O) in two versions of the Whole Atmosphere Chemistry-Climate Model (WACCM) by comparing them with measurements from four Fourier transform infrared (FTIR) ground-based instruments, the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS), and with a chemistry-transport model (CTM) driven by four different reanalyses. The limited sensitivity of the FTIR instruments can hide negative N2O trends in the mid-stratosphere because of the large increase in the lowermost stratosphere. When applying ACE-FTS measurement sampling on model datasets, the reanalyses from the European Center for Medium Range Weather Forecast (ECMWF) compare best with ACE-FTS, but the N2O trends are consistently exaggerated. The N2O trends obtained with WACCM disagree with those obtained from ACE-FTS, but the new WACCM version performs better than the previous above the Southern Hemisphere in the stratosphere. Model sensitivity tests show that the decadal N2O trends reflect changes in the stratospheric transport. We further investigate the N2O Transformed Eulerian Mean (TEM) budget in WACCM and in the CTM simulation driven by the latest ECMWF reanalysis. The TEM analysis shows that enhanced advection affects the stratospheric N2O trends in the Tropics. While no ideal observational dataset currently exists, this model study of N2O trends still provides new insights about the BDC and its changes because of the contribution from relevant sensitivity tests and the TEM analysis.

©2019. American Geophysical Union. All Rights Reserved. It has recently been recognized that, in addition to greenhouse gases, anthropogenic emissions of ozone-depleting substances (ODS) can induce long-term trends in the Brewer-Dobson circulation (BDC). Several studies have shown that a substantial fraction of the residual circulation acceleration over the last decades of the twentieth century can be attributed to increasing ODS. Here the mechanisms of this influence are examined, comparing model runs to reanalysis data and evaluating separately the residual circulation and mixing contributions to the mean age of air trends. The effects of ozone depletion in the Antarctic lower stratosphere are found to dominate the ODS impact on the BDC, while the direct radiative impact of these substances is negligible over the period of study. We find qualitative agreement in austral summer BDC trends between model and reanalysis data and show that ODS are the main driver of both residual circulation and isentropic mixing trends over the last decades of the twentieth century. Moreover, aging by isentropic mixing is shown to play a key role on ODS-driven age of air trends.

The extreme disruptions of the wintertime stratospheric circulation during sudden stratospheric warmings (SSW) have large effects on tracer concentrations through alterations in transport. This study analyzes the changes in residual circulation and isentropic mixing associated with SSWs, by performing composites using reanalysis (European Centre for Medium‐Range Weather Forecasts Re‐Analysis Interim) and simulations of the Whole Atmosphere Community Climate Model. The advective Brewer‐Dobson circulation accelerates around 15 days prior to the wind reversal at 60°N, 10 hPa during the onset of SSWs. Soon afterward, it decelerates, leading to reduced advective transport into the vortex and descent over the pole, which persist for more than 2 months below 30 hPa. The isentropic mixing has a distinct signature in altitude: It is enhanced at the central date of the SSW in the midstratosphere (about 10 hPa or 800 K), and this signal is delayed and more persistent at lower altitudes. It is shown that sufficiently deep SSWs (particularly those related to Polar‐night Jet Oscillation events) have a stronger response in the Brewer‐Dobson circulation and mixing. In particular, both the polar downwelling and the tropical upwelling are anomalously weak in the lower stratosphere for 90 days after the onset of Polar‐night Jet Oscillation events. The redistribution of potential vorticity during the life cycle of SSWs is discussed due to its relevance for the stratospheric circulation. It is shown that the diffusive flux of potential vorticity, calculated in equivalent latitude coordinates, remains anomalously high in the lower stratosphere, a feature that is not seen in more conventional advective eddy fluxes across latitude circles.

Sudden stratospheric warmings (SSWs) are the main source of intra-seasonal and interannual variability in the extratropical stratosphere. The profound alterations to the stratospheric circulation that accompany such events produce rapid changes in the atmospheric composition. The goal of this study is to deepen our understanding of the dynamics that control changes of Arctic ozone during the life cycle of SSWs, providing a quantitative analysis of advective transport and mixing. We use output from four ensemble members (60 years each) of the Whole Atmospheric Community Climate Model version 4 performed for the Chemistry Climate Model Initiative and also use reanalysis and satellite data for validation purposes. The composite evolution of ozone displays positive mixing ratio anomalies of up to 0.5–0.6 ppmv above 550 K (∼ 50 hPa) around the central warming date and negative anomalies below (−0.2 to −0.3 ppmv), consistently in observations, reanalysis, and the model. Our analysis shows a clear temporal offset between ozone eddy transport and diffusive ozone fluxes. The initial changes in ozone are mainly driven by isentropic eddy fluxes linked to enhanced wave drag responsible for the SSW. The recovery of climatological values in the aftermath of SSWs is slower in the lower than in the upper stratosphere and is driven by the competing effects of cross-isentropic motions (which work towards the recovery) and isentropic irreversible mixing (which delays the recovery). These features are enhanced in strength and duration during sufficiently deep SSWs, particularly those followed by polar-night jet oscillation (PJO) events. It is found that SSW-induced ozone concentration anomalies below 600 K (∼ 40 hPa), as well as total column estimates, persist around 1 month longer in PJO than in non-PJO warmings.

The stratospheric ozone layer shields surface life from harmful ultraviolet radiation. Following the Montreal Protocol ban on long-lived ozone-depleting substances (ODSs), rapid depletion of total column ozone (TCO) ceased in the late 1990s, and ozone above 32 km is now clearly recovering. However, there is still no confirmation of TCO recovery, and evidence has emerged that ongoing quasi-global (60∘ S–60∘ N) lower stratospheric ozone decreases may be responsible, dominated by low latitudes (30∘ S–30∘ N). Chemistry–climate models (CCMs) used to project future changes predict that lower stratospheric ozone will decrease in the tropics by 2100 but not at mid-latitudes (30–60∘). Here, we show that CCMs display an ozone decline similar to that observed in the tropics over 1998–2016, likely driven by an increase in tropical upwelling. On the other hand, mid-latitude lower stratospheric ozone is observed to decrease, while CCMs that specify real-world historical meteorological fields instead show an increase up to present day. However, these cannot be used to simulate future changes; we demonstrate here that free-running CCMs used for projections also show increases. Despite opposing lower stratospheric ozone changes, which should induce opposite temperature trends, CCMs and observed temperature trends agree; we demonstrate that opposing model–observation stratospheric water vapour (SWV) trends, and their associated radiative effects, explain why temperature changes agree in spite of opposing ozone trends. We provide new evidence that the observed mid-latitude trends can be explained by enhanced mixing between the tropics and extratropics. We further show that the temperature trends are consistent with the observed mid-latitude ozone decrease. Together, our results suggest that large-scale circulation changes expected in the future from increased greenhouse gases (GHGs) may now already be underway but that most CCMs do not simulate mid-latitude ozone layer changes well. H, Atmospheric Remote Sensing