ALBERT

Description: Various observation-based datasets have confirmed positive zonal mean column ozone trends at midlatitudes as a result of the successful implementation of the Montreal Protocol. However, there is still uncertainty about the longitudinal variation of these trends and the direction and magnitude of ozone changes at low latitudes. Here, we use the extended Copernicus Climate Change Service (C3S) dataset (1979–2017) to investigate the long-term variations in total column ozone (TCO) over the Tibetan Plateau (TP) for different seasons. We use piecewise linear trend (PWLT) and equivalent effective stratospheric chlorine loading (EESC)-based multivariate regression models with various proxies to attribute the influence of dynamical and chemical processes on the TCO variability. We also compare the seasonal behaviour of the relative total ozone low (TOL) over the TP with the zonal mean at the same latitude. Both regression models show that the TP column ozone trends change from negative trends from 1979 to 1996 to small positive trends from 1997 to 2017, although the later positive trend based on PWLT is not statistically significant. The wintertime positive trend starting from 1997 is larger than that in summer, but both seasonal TP recovery rates are smaller than the zonal means over the same latitude band. For TP column ozone, both regression models suggest that the geopotential height at 150 hPa (GH150) is a more suitable and realistic dynamical proxy compared to a surface temperature proxy used in some previous studies. Our analysis also shows that the wintertime GH150 plays an important role in determining summertime TCO over the TP through persistence of the ozone signal. For the zonal mean column ozone at this latitude, the quasi-biennial oscillation (QBO) is nonetheless the dominant dynamical proxy. We also use a 3-D chemical transport model to diagnose the contributions of different proxies for the TP region. The role of GH150 variability is illustrated by using two sensitivity experiments with repeating dynamics of 2004 and 2008. The simulated ozone profiles clearly show that wintertime TP ozone concentrations are largely controlled by tropics to midlatitude pathways, whereas in summer variations associated with tropical processes play an important role. These model results confirm that the long-term trends of TCO over the TP are dominated by different processes in winter and summer. The different TP recovery rates relative to the zonal means at the same latitude band are largely determined by wintertime dynamical processes.

Description: Despite the recently reported beginning of a recovery in global stratospheric ozone (O3), an unexpected O3 decline in the tropical mid-stratosphere (around 30–35 km altitude) was observed in satellite measurements during the first decade of the 21st century. We use SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY) measurements for the period 2004–2012 to confirm the significant O3 decline. The SCIAMACHY observations show that the decrease in O3 is accompanied by an increase in NO2. To reveal the causes of these observed O3 and NO2 changes, we performed simulations with the TOMCAT 3-D chemistry-transport model (CTM) using different chemical and dynamical forcings. For the 2004–2012 time period, the TOMCAT simulations reproduce the SCIAMACHY-observed O3 decrease and NO2 increase in the tropical mid-stratosphere. The simulations suggest that the positive changes in NO2 (around 7 % decade−1) are due to similar positive changes in reactive odd nitrogen (NOy), which are a result of a longer residence time of the source gas N2O and increased production via N2O + O(1D). The model simulations show a negative change of 10 % decade−1 in N2O that is most likely due to variations in the deep branch of the Brewer–Dobson Circulation (BDC). Interestingly, modelled annual mean “age of air” (AoA) does not show any significant changes in transport in the tropical mid-stratosphere during 2004–2012. However, further analysis of model results demonstrates significant seasonal variations. During the autumn months (September–October) there are positive AoA changes that imply transport slowdown and a longer residence time of N2O allowing for more conversion to NOy, which enhances O3 loss. During winter months (January–February) there are negative AoA changes, indicating faster N2O transport and less NOy production. Although the variations in AoA over a year result in a statistically insignificant linear change, non-linearities in the chemistry–transport interactions lead to a statistically significant negative N2O change.

Description: Stratospheric ozone loss inside the Arctic polar vortex for the winters between 2004–2005 and 2012–2013 has been quantified using measurements from the space-borne Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS). For the first time, an evaluation has been performed of six different ozone loss estimation methods based on the same single observational dataset to determine the Arctic ozone loss (mixing ratio loss profiles and the partial-column ozone losses between 380 and 550 K). The methods used are the tracer-tracer correlation, the artificial tracer correlation, the average vortex profile descent, and the passive subtraction with model output from both Lagrangian and Eulerian chemical transport models (CTMs). For the tracer-tracer, the artificial tracer, and the average vortex profile descent approaches, various tracers have been used that are also measured by ACE-FTS. From these seven tracers investigated (CH4, N2O, HF, OCS, CFC-11, CFC-12, and CFC-113), we found that CH4, N2O, HF, and CFC-12 are the most suitable tracers for investigating polar stratospheric ozone depletion with ACE-FTS v3.5. The ozone loss estimates (in terms of the mixing ratio as well as total column ozone) are generally in good agreement between the different methods and among the different tracers. However, using the average vortex profile descent technique typically leads to smaller maximum losses (by approximately 15–30 DU) compared to all other methods. The passive subtraction method using output from CTMs generally results in slightly larger losses compared to the techniques that use ACE-FTS measurements only. The ozone loss computed, using both measurements and models, shows the greatest loss during the 2010–2011 Arctic winter. For that year, our results show that maximum ozone loss (2.1–2.7 ppmv) occurred at 460 K. The estimated partial-column ozone loss inside the polar vortex (between 380 and 550 K) using the different methods is 66–103, 61–95, 59–96, 41–89, and 85–122 DU for March 2005, 2007, 2008, 2010, and 2011, respectively. Ozone loss is difficult to diagnose for the Arctic winters during 2005–2006, 2008–2009, 2011–2012, and 2012–2013, because strong polar vortex disturbance or major sudden stratospheric warming events significantly perturbed the polar vortex, thereby limiting the number of measurements available for the analysis of ozone loss.

Description: We have used satellite observations and a simulation from the TOMCAT chemistry transport model (CTM) to investigate the influence of the well-known wintertime North Atlantic Oscillation (NAO) on European tropospheric composition. Under the positive phase of the NAO (NAO-high), strong westerlies tend to enhance transport of European pollution (e.g. nitrogen oxides, NOx; carbon monoxide, CO) away from anthropogenic source regions. In contrast, during the negative phase of the NAO (NAO-low), more stable meteorological conditions lead to a build-up of pollutants over these regions relative to the wintertime average pollution levels. However, the secondary pollutant ozone shows the opposite signal of larger values during NAO-high. NAO-high introduces Atlantic ozone-enriched air into Europe, while under NAO-low westerly transport of ozone is reduced, yielding lower values over Europe. Furthermore, ozone concentrations are also decreased by chemical loss through the reaction with accumulated primary pollutants such as nitric oxide (NO) in NAO-low. Peroxyacetyl nitrate (PAN) in the upper troposphere–lower stratosphere (UTLS) peaks over Iceland and southern Greenland in NAO-low, between 200 and 100 hPa, consistent with the trapping by an anticyclone at this altitude. Model simulations show that enhanced PAN over Iceland and southern Greenland in NAO-low is associated with vertical transport of polluted air from the mid-troposphere into the UTLS. Overall, this work shows that NAO circulation patterns are an important governing factor for European wintertime composition and air pollution.

Description: Ozone fields simulated for the first phase of the Chemistry-Climate Model Initiative (CCMI-1) will be used as forcing data in the 6th Coupled Model Intercomparison Project. Here we assess, using reference and sensitivity simulations produced for CCMI-1, the suitability of CCMI-1 model results for this process, investigating the degree of consistency amongst models regarding their responses to variations in individual forcings. We consider the influences of methane, nitrous oxide, a combination of chlorinated or brominated ozone-depleting substances, and a combination of carbon dioxide and other greenhouse gases. We find varying degrees of consistency in the models' responses in ozone to these individual forcings, including some considerable disagreement. In particular, the response of total-column ozone to these forcings is less consistent across the multi-model ensemble than profile comparisons. We analyse how stratospheric age of air, a commonly used diagnostic of stratospheric transport, responds to the forcings. For this diagnostic we find some salient differences in model behaviour, which may explain some of the findings for ozone. The findings imply that the ozone fields derived from CCMI-1 are subject to considerable uncertainties regarding the impacts of these anthropogenic forcings. We offer some thoughts on how to best approach the problem of generating a consensus ozone database from a multi-model ensemble such as CCMI-1.

Description: 〉We analyse simulations performed for the Chemistry-Climate Model Initiative (CCMI) to estimate the return dates of the stratospheric ozone layer from depletion caused by anthropogenic stratospheric chlorine and bromine. We consider a total of 155 simulations from 20 models, including a range of sensitivity studies which examine the impact of climate change on ozone recovery. For the control simulations (unconstrained by nudging towards analysed meteorology) there is a large spread (±20 DU in the global average) in the predictions of the absolute ozone column. Therefore, the model results need to be adjusted for biases against historical data. Also, the interannual variability in the model results need to be smoothed in order to provide a reasonably narrow estimate of the range of ozone return dates. Consistent with previous studies, but here for a Representative Concentration Pathway (RCP) of 6.0, these new CCMI simulations project that global total column ozone will return to 1980 values in 2049 (with a 1σ uncertainty of 2043–2055). At Southern Hemisphere mid-latitudes column ozone is projected to return to 1980 values in 2045 (2039–2050), and at Northern Hemisphere mid-latitudes in 2032 (2020–2044). In the polar regions, the return dates are 2060 (2055–2066) in the Antarctic in October and 2034 (2025–2043) in the Arctic in March. The earlier return dates in the Northern Hemisphere reflect the larger sensitivity to dynamical changes. Our estimates of return dates are later than those presented in the 2014 Ozone Assessment by approximately 5–17 years, depending on the region, with the previous best estimates often falling outside of our uncertainty range. In the tropics only around half the models predict a return of ozone to 1980 values, around 2040, while the other half do not reach the 1980 value. All models show a negative trend in tropical total column ozone towards the end of the 21st century. The CCMI models generally agree in their simulation of the time evolution of stratospheric chlorine and bromine, which are the main drivers of ozone loss and recovery. However, there are a few outliers which show that the multi-model mean results for ozone recovery are not as tightly constrained as possible. Throughout the stratosphere the spread of ozone return dates to 1980 values between models tends to correlate with the spread of the return of inorganic chlorine to 1980 values. In the upper stratosphere, greenhouse gas-induced cooling speeds up the return by about 10–20 years. In the lower stratosphere, and for the column, there is a more direct link in the timing of the return dates of ozone and chlorine, especially for the large Antarctic depletion. Comparisons of total column ozone between the models is affected by different predictions of the evolution of tropospheric ozone within the same scenario, presumably due to differing treatment of tropospheric chemistry. Therefore, for many scenarios, clear conclusions can only be drawn for stratospheric ozone columns rather than the total column. As noted by previous studies, the timing of ozone recovery is affected by the evolution of N2O and CH4. However, quantifying the effect in the simulations analysed here is limited by the few realisations available for these experiments compared to internal model variability. The large increase in N2O given in RCP 6.0 extends the ozone return globally by ∼ 15 years relative to N2O fixed at 1960 abundances, mainly because it allows tropical column ozone to be depleted. The effect in extratropical latitudes is much smaller. The large increase in CH4 given in the RCP 8.5 scenario compared to RCP 6.0 also lengthens ozone return by ∼ 15 years, again mainly through its impact in the tropics. Overall, our estimates of ozone return dates are uncertain due to both uncertainties in future scenarios, in particular those of greenhouse gases, and uncertainties in models. The scenario uncertainty is small in the short term but increases with time, and becomes large by the end of the century. There are still some model–model differences related to well-known processes which affect ozone recovery. Efforts need to continue to ensure that models used for assessment purposes accurately represent stratospheric chemistry and the prescribed scenarios of ozone-depleting substances, and only those models are used to calculate return dates. For future assessments of single forcing or combined effects of CO2, CH4, and N2O on the stratospheric column ozone return dates, this work suggests that it is more important to have multi-member (at least three) ensembles for each scenario from every established participating model, rather than a large number of individual models.

Description: The enhancement of the stratospheric aerosol layer by volcanic eruptions induces a complex set of responses causing global and regional climate effects on a broad range of timescales. Uncertainties exist regarding the climatic response to strong volcanic forcing identified in coupled climate simulations that contributed to the fifth phase of the Coupled Model Intercomparison Project (CMIP5). In order to better understand the sources of these model diversities, the Model Intercomparison Project on the climatic response to Volcanic forcing (VolMIP) has defined a coordinated set of idealized volcanic perturbation experiments to be carried out in alignment with the CMIP6 protocol. VolMIP provides a common stratospheric aerosol data set for each experiment to minimize differences in the applied volcanic forcing. It defines a set of initial conditions to assess how internal climate variability contributes to determining the response. VolMIP will assess to what extent volcanically forced responses of the coupled ocean–atmosphere system are robustly simulated by state-of-the-art coupled climate models and identify the causes that limit robust simulated behavior, especially differences in the treatment of physical processes. This paper illustrates the design of the idealized volcanic perturbation experiments in the VolMIP protocol and describes the common aerosol forcing input data sets to be used.

Description: We present an overview of state-of-the-art chemistry–climate and chemistry transport models that are used within phase 1 of the Chemistry–Climate Model Initiative (CCMI-1). The CCMI aims to conduct a detailed evaluation of participating models using process-oriented diagnostics derived from observations in order to gain confidence in the models' projections of the stratospheric ozone layer, tropospheric composition, air quality, where applicable global climate change, and the interactions between them. Interpretation of these diagnostics requires detailed knowledge of the radiative, chemical, dynamical, and physical processes incorporated in the models. Also an understanding of the degree to which CCMI-1 recommendations for simulations have been followed is necessary to understand model responses to anthropogenic and natural forcing and also to explain inter-model differences. This becomes even more important given the ongoing development and the ever-growing complexity of these models. This paper also provides an overview of the available CCMI-1 simulations with the aim of informing CCMI data users.

Description: Despite the recently reported beginning of a recovery in global stratospheric ozone (O3), an unexpected O3 decline in the tropical mid-stratosphere (around 30–35km altitude) was observed in satellite measurements during the first decade of the 21st century. We use SCanning Imaging Absorption SpectroMeter for Atmospheric CHartographY (SCIAMACHY) measurements for the period 2004–2012 to confirm the significant O3 decline. The SCIAMACHY observations also show that the decrease in O3 is accompanied by an increase in NO2. To reveal the causes of these observed O3 and NO2 changes, we performed simulations with the TOMCAT 3D Chemistry-Transport Model (CTM) using different chemical and dynamical forcings. For the 2004–2012 time period, the TOMCAT simulations reproduce the SCIAMACHY-observed O3 decrease and NO2 increase in the tropical mid-stratosphere. The simulations suggest that the positive changes in NO2 (around 7% per decade) are due to similar positive changes in reactive odd nitrogen (NOy), which are a result of a longer residence time of the source gas N2O and increased production via N2O+O(1D). The model simulations show a negative change of 10% per decade in N2O that is most likely due to variations in the deep branch of the Brewer-Dobson Circulation (BDC). Interestingly, modelled annual mean age-of-air (AoA) does not show any significant changes in the transport in the tropical mid-stratosphere during 2004–2012. However, further analysis of model results demonstrate significant seasonal variations. During the autumn months (September–October) there are positive AoA changes, that imply transport slowdown and a longer residence time of N2O allowing larger conversion to NOy which enhances O3 loss. During winter months (January–February) there are negative AoA changes, indicating faster N2O transport and less NOy production. Although the changes in AoA cancel out when averaging over the year, non-linearities in the chemistry-transport interactions mean that the net negative N2O change remains.

Description: We have used satellite observations and a simulation from the TOMCAT chemistry transport model (CTM) to investigate the influence of the well-known winter-time North Atlantic Oscillation (NAO) on European tropospheric composition. Under the positive phase of the NAO (NAO+), strong westerlies tend to enhance transport of European pollution (e.g. nitrogen oxides, NOx, carbon monoxide, CO) away from anthropogenic source regions. In contrast, during the negative phase of the NAO (NAO−), more stable meteorological conditions lead to a build up of pollutants over these regions, relative to the winter-time average pollution levels. However, the secondary pollutant ozone shows the opposite signal of larger values during NAO+. NAO+ introduces Atlantic ozone-enriched air into Europe while under NAO− westerly transport of ozone is reduced yielding lower values over Europe. Furthermore, ozone concentrations are also decreased by chemical loss through the reaction with accumulated primary pollutants such as nitric oxide (NO) in NAO−. Peroxyacetyl nitrate (PAN), in the upper troposphere-lower stratosphere (UTLS) peaks over Iceland/Southern Greenland in NAO−, between 200–100 hPa, consistent with the trapping by an anticyclone at this altitude. Model simulations show enhanced PAN over Iceland/Southern Greenland in NAO− is associated with vertical transport of polluted air from the troposphere into the UTLS. Overall, this work shows that NAO circulation patterns are an important governing factor for European winter-time composition and air pollution.