Attribution of ozone changes to dynamical and chemical processes in CCMs and CTMs

Chemistry-climate models (CCMs) are commonly used to simulate the past and future development of Earth's ozone layer. The fully coupled chemistry schemes calculate the chemical production and destruction of ozone interactively and ozone is transported by the simulated atmospheric flow. Due to the complexity of the processes acting on ozone it is not straightforward to disentangle the influence of individual processes on the temporal development of ozone concentrations. A method is introduced here that quantifies the influence of chemistry and transport on ozone concentration changes and that is easily implemented in CCMs and chemistry-transport models (CTMs). In this method, ozone tendencies (i.e. the time rate of change of ozone) are partitioned into a contribution from ozone production and destruction (chemistry) and a contribution from transport of ozone (dynamics). The influence of transport on ozone in a specific region is further divided into export of ozone out of that region and import of ozone from elsewhere into that region. For this purpose, a diagnostic is used that disaggregates the ozone mixing ratio field into 9 separate fields according to in which of 9 predefined regions of the atmosphere the ozone originated. With this diagnostic the ozone mass fluxes between these regions are obtained. Furthermore, this method is used here to attribute long-term changes in ozone to chemistry and transport. The relative change in ozone from one period to another that is due to changes in production or destruction rates, or due to changes in import or export of ozone, are quantified. As such, the diagnostics introduced here can be used to attribute changes in ozone on monthly, interannual and long-term time-scales to the responsible mechanisms. Results from a CCM simulation are shown here as examples, with the main focus of the paper being on introducing the method

The influence of future changes in springtime Arctic ozone on stratospheric and surface climate

Stratospheric ozone is expected to recover by the mid-century due to the success of the Montreal Protocol in regulating the emission of ozone-depleting substances (ODSs). In the Arctic, ozone abundances are projected to surpass historical levels due to the combined effect of decreasing ODSs and elevated greenhouse gases (GHGs). While long-term changes in stratospheric ozone have been shown to be a major driver of future surface climate in the Southern Hemisphere during summertime, the dynamical and climatic impacts of elevated ozone levels in the Arctic have not been investigated. In this study, we use two chemistry climate models (the SOlar Climate Ozone Links – Max Planck Ocean Model (SOCOL-MPIOM) and the Community Earth System Model – Whole Atmosphere Community Climate Model (CESM-WACCM)) to assess the climatic impacts of future changes in Arctic ozone on stratospheric dynamics and surface climate in the Northern Hemisphere (NH) during the 21st century. Under the high-emission scenario (RCP8.5) examined in this work, Arctic ozone returns to pre-industrial levels by the middle of the century. Thereby, the increase in Arctic ozone in this scenario warms the lower Arctic stratosphere; reduces the strength of the polar vortex, advancing its breakdown; and weakens the Brewer–Dobson circulation. The ozone-induced changes in springtime generally oppose the effects of GHGs on the polar vortex. In the troposphere, future changes in Arctic ozone induce a negative phase of the Arctic Oscillation, pushing the jet equatorward over the North Atlantic. These impacts of future ozone changes on NH surface climate are smaller than the effects of GHGs, but they are remarkably robust among the two models employed in this study, canceling out a portion of the GHG effects (up to 20 % over the Arctic). In the stratosphere, Arctic ozone changes cancel out a much larger fraction of the GHG-induced signal (up to 50 %–100 %), resulting in no overall change in the projected springtime stratospheric northern annular mode and a reduction in the GHG-induced delay of vortex breakdown of around 15 d. Taken together, our results indicate that future changes in Arctic ozone actively shape the projected changes in the stratospheric circulation and their coupling to the troposphere, thereby playing an important and previously unrecognized role as a driver of the large-scale atmospheric circulation response to climate change.</p

Global long-term monitoring of the ozone layer - a prerequisite for predictions

Although the Montreal Protocol now controls the production and emission of ozone depleting substances, the timing of ozone recovery is unclear. There are many other factors affecting the ozone layer, in particular climate change is expected to modify the speed of re-creation of the ozone layer. Therefore, long-term observations are needed to monitor the further evolution of the stratospheric ozone layer. Measurements from satellite instruments provide global coverage and are supplementary to selective ground-based observations. The combination of data derived from different space-borne instruments is needed to produce homogeneous and consistent long-term data records. They are required for robust investigations including trend analysis. For the first time global total ozone columns from three European satellite sensors GOME (ERS-2), SCIAMACHY (ENVISAT), and GOME-2 (METOP-A) are combined and added up to a continuous time series starting in June 1995. On the one hand it is important to monitor the consequences of the Montreal Protocol and its amendments; on the other hand multi-year observations provide the basis for the evaluation of numerical models describing atmospheric processes, which are also used for prognostic studies to assess the future development. This paper gives some examples of how to use satellite data products to evaluate model results with respective data derived from observations, and to disclose the abilities and deficiencies of atmospheric models. In particular, multi-year mean values derived from the Chemistry-Climate Model E39C-A are used to check climatological values and the respective standard deviations

Weakening of springtime Arctic ozone depletion with climate change

In the Arctic stratosphere, the combination of chemical ozone depletion by halogenated ozone-depleting substances (hODSs) and dynamic fluctuations can lead to severe ozone minima. These Arctic ozone minima are of great societal concern due to their health and climate impacts. Owing to the success of the Montreal Protocol, hODSs in the stratosphere are gradually declining, resulting in a recovery of the ozone layer. On the other hand, continued greenhouse gas (GHG) emissions cool the stratosphere, possibly enhancing the formation of polar stratospheric clouds (PSCs) and, thus, enabling more efficient chemical ozone destruction. Other processes, such as the acceleration of the Brewer–Dobson circulation, also affect stratospheric temperatures, further complicating the picture. Therefore, it is currently unclear whether major Arctic ozone minima will still occur at the end of the 21st century despite decreasing hODSs. We have examined this question for different emission pathways using simulations conducted within the Chemistry-Climate Model Initiative (CCMI-1 and CCMI-2022) and found large differences in the models' ability to simulate the magnitude of ozone minima in the present-day climate. Models with a generally too-cold polar stratosphere (cold bias) produce pronounced ozone minima under present-day climate conditions because they simulate more PSCs and, thus, high concentrations of active chlorine species (ClOx). These models predict the largest decrease in ozone minima in the future. Conversely, models with a warm polar stratosphere (warm bias) have the smallest sensitivity of ozone minima to future changes in hODS and GHG concentrations. As a result, the scatter among models in terms of the magnitude of Arctic spring ozone minima will decrease in the future. Overall, these results suggest that Arctic ozone minima will become weaker over the next decades, largely due to the decline in hODS abundances. We note that none of the models analysed here project a notable increase of ozone minima in the future. Stratospheric cooling caused by increasing GHG concentrations is expected to play a secondary role as its effect in the Arctic stratosphere is weakened by opposing radiative and dynamical mechanisms

Inter-model comparison of global hydroxyl radical (OH) distributions and their impact on atmospheric methane over the 2000–2016 period

The modeling study presented here aims to estimate how uncertainties in global hydroxyl radical (OH) distributions, variability, and trends may contribute to resolving discrepancies between simulated and observed methane (CH4) changes since 2000. A multi-model ensemble of 14 OH fields was analyzed and aggregated into 64 scenarios to force the offline atmospheric chemistry transport model LMDz (Laboratoire de Meteorologie Dynamique) with a standard CH4 emission scenario over the period 2000–2016. The multi-model simulated global volume-weighted tropospheric mean OH concentration ([OH]) averaged over 2000–2010 ranges between 8:7*10^5 and 12:8*10^5 molec cm-3. The inter-model differences in tropospheric OH burden and vertical distributions are mainly determined by the differences in the nitrogen oxide (NO) distributions, while the spatial discrepancies between OH fields are mostly due to differences in natural emissions and volatile organic compound (VOC) chemistry. From 2000 to 2010, most simulated OH fields show an increase of 0.1–0:3*10^5 molec cm-3 in the tropospheric mean [OH], with year-to-year variations much smaller than during the historical period 1960–2000. Once ingested into the LMDz model, these OH changes translated into a 5 to 15 ppbv reduction in the CH4 mixing ratio in 2010, which represents 7%–20% of the model-simulated CH4 increase due to surface emissions. Between 2010 and 2016, the ensemble of simulations showed that OH changes could lead to a CH4 mixing ratio uncertainty of > 30 ppbv. Over the full 2000–2016 time period, using a common stateof- the-art but nonoptimized emission scenario, the impact of [OH] changes tested here can explain up to 54% of the gap between model simulations and observations. This result emphasizes the importance of better representing OH abundance and variations in CH4 forward simulations and emission optimizations performed by atmospheric inversions

Evaluating the relationship between interannual variations in the Antarctic ozone hole and Southern Hemisphere surface climate in chemistry-climate models

Studies have recently reported statistically significant relationships between observed year-to-year spring Antarctic ozone variability and the Southern Hemisphere Annular Mode and surface temperatures in spring-summer. This study investigates whether current chemistry-climate models (CCMs) can capture these relationships, in particular, the connection between November total column ozone (TCO) and Australian summer surface temperatures, where years with anomalously high TCO over the Antarctic polar cap tend to be followed by warmer summers. The interannual ozone-temperature teleconnection is examined over the historical period in the observations and simulations from the Whole Atmosphere Community Climate Model (WACCM) and nine other models participating in the Chemistry-Climate Model Initiative (CCMI). There is a systematic difference between the WACCM experiments forced with prescribed observed sea surface temperatures (SSTs) and those with an interactive ocean. Strong correlations between TCO and Australian temperatures are only obtained for the uncoupled experiment, suggesting that the SSTs could be important for driving both variations in Australian temperatures and the ozone hole, with no causal link between the two. Other CCMI models also tend to capture this relationship with more fidelity when driven by observed SSTs, though additional research and targeted modelling experiments are required to determine causality and further explore the role of model biases and observational uncertainty. The results indicate that CCMs can reproduce the relationship between spring ozone and summer Australian climate reported in observational studies, suggesting that incorporating ozone variability could improve seasonal predictions, however more work is required to understand the difference between the coupled and uncoupled simulations

Evaluating the relationship between interannual variations in the Antarctic ozone hole and Southern Hemisphere surface climate in chemistry-climate models

Studies have recently reported statistically significant relationships between observed year-to-year spring Antarctic ozone variability and the Southern Hemisphere Annular Mode and surface temperatures in spring-summer. This study investigates whether current chemistry-climate models (CCMs) can capture these relationships, in particular, the connection between November total column ozone (TCO) and Australian summer surface temperatures, where years with anomalously high TCO over the Antarctic polar cap tend to be followed by warmer summers. The interannual ozone-temperature teleconnection is examined over the historical period in the observations and simulations from the Whole Atmosphere Community Climate Model (WACCM) and nine other models participating in the Chemistry-Climate Model Initiative (CCMI). There is a systematic difference between the WACCM experiments forced with prescribed observed sea surface temperatures (SSTs) and those with an interactive ocean. Strong correlations between TCO and Australian temperatures are only obtained for the uncoupled experiment, suggesting that the SSTs could be important for driving both variations in Australian temperatures and the ozone hole, with no causal link between the two. Other CCMI models also tend to capture this relationship with more fidelity when driven by observed SSTs, though additional research and targeted modelling experiments are required to determine causality and further explore the role of model biases and observational uncertainty. The results indicate that CCMs can reproduce the relationship between spring ozone and summer Australian climate reported in observational studies, suggesting that incorporating ozone variability could improve seasonal predictions, however more work is required to understand the difference between the coupled and uncoupled simulations