ALBERT

Description: The stratospheric age of air (AoA) is a useful measure of the overall capabilities of a general circulation model (GCM) to simulate stratospheric transport. Previous studies have reported a large spread in the simulation of AoA by GCMs and coupled chemistry–climate models (CCMs). Compared to observational estimates, simulated AoA is mostly too low. Here we attempt to untangle the processes that lead to the AoA differences between the models and between models and observations. AoA is influenced by both mean transport by the residual circulation and two-way mixing; we quantify the effects of these processes using data from the CCM inter-comparison projects CCMVal-2 (Chemistry–Climate Model Validation Activity 2) and CCMI-1 (Chemistry–Climate Model Initiative, phase 1). Transport along the residual circulation is measured by the residual circulation transit time (RCTT). We interpret the difference between AoA and RCTT as additional aging by mixing. Aging by mixing thus includes mixing on both the resolved and subgrid scale. We find that the spread in AoA between the models is primarily caused by differences in the effects of mixing and only to some extent by differences in residual circulation strength. These effects are quantified by the mixing efficiency, a measure of the relative increase in AoA by mixing. The mixing efficiency varies strongly between the models from 0.24 to 1.02. We show that the mixing efficiency is not only controlled by horizontal mixing, but by vertical mixing and vertical diffusion as well. Possible causes for the differences in the models' mixing efficiencies are discussed. Differences in subgrid-scale mixing (including differences in advection schemes and model resolutions) likely contribute to the differences in mixing efficiency. However, differences in the relative contribution of resolved versus parameterized wave forcing do not appear to be related to differences in mixing efficiency or AoA.

Description: Sulfate geoengineering (SG), made by sustained injection of SO2 in the tropical lower stratosphere, may impact the CH4 abundance through several photochemical mechanisms affecting tropospheric OH and hence the methane lifetime. (a) The reflection of incoming solar radiation increases the planetary albedo and cools the surface, with a tropospheric H2O decrease. (b) The tropospheric UV budget is upset by the additional aerosol scattering and stratospheric ozone changes: the net effect is meridionally not uniform, with a net decrease in the tropics, thus producing less tropospheric O(1D). (c) The extratropical downwelling motion from the lower stratosphere tends to increase the sulfate aerosol surface area density available for heterogeneous chemical reactions in the mid-to-upper troposphere, thus reducing the amount of NOx and O3 production. (d) The tropical lower stratosphere is warmed by solar and planetary radiation absorption by the aerosols. The heating rate perturbation is highly latitude dependent, producing a stronger meridional component of the Brewer–Dobson circulation. The net effect on tropospheric OH due to the enhanced stratosphere–troposphere exchange may be positive or negative depending on the net result of different superimposed species perturbations (CH4, NOy, O3, SO4) in the extratropical upper troposphere and lower stratosphere (UTLS). In addition, the atmospheric stabilization resulting from the tropospheric cooling and lower stratospheric warming favors an additional decrease of the UTLS extratropical CH4 by lowering the horizontal eddy mixing. Two climate–chemistry coupled models are used to explore the above radiative, chemical and dynamical mechanisms affecting CH4 transport and lifetime (ULAQ-CCM and GEOSCCM). The CH4 lifetime may become significantly longer (by approximately 16 %) with a sustained injection of 8 Tg-SO2 yr−1 starting in the year 2020, which implies an increase of tropospheric CH4 (200 ppbv) and a positive indirect radiative forcing of sulfate geoengineering due to CH4 changes (+0.10 W m−2 in the 2040–2049 decade and +0.15 W m−2 in the 2060–2069 decade).

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: We have used total ozone columns and vertical profiles of ozone and temperature from 11 coupled Chemistry-Climate Models (CCMs) to project future solar ultraviolet radiation levels at the surface in the 21st century. The CCM simulations are used as input to a radiative transfer model for the simulation of the corresponding future UV irradiance levels under cloud free conditions, presented here as time series of monthly erythemal irradiance received at the surface during local noon covering the period 1960 to 2100. Starting from the first decade of the 21st century, the surface erythemal irradiance decreases globally as a result of the projected ozone recovery, at rates which are larger in the first half of the 21st century, compared to the period up to 2100. The magnitude of these decreases varies with latitude and is more pronounced at areas where ozone has been depleted most considerably after 1980. Over midlatitudes surface erythemal irradiance decreases between 5 and 15% by 2100 relative to 2000, while at the southern high latitudes these changes are twice as much. Climate change may affect future cloudiness, surface reflectivity and tropospheric aerosol loading, the effects of which are not included in this study. Therefore, the actual changes in future UV radiation are likely to change accordingly in the areas affected.

Description: In this work we focus on the direct radiative forcing (RF) of black carbon (BC) and sulphuric acid particles emitted by future supersonic aircraft, as well as on the ozone RF due to changes produced by emissions of both gas species (NOx, H2O) and aerosol particles capable of affecting stratospheric ozone chemistry. Heterogeneous chemical reactions on the surface of sulphuric acid stratospheric particles (SSA-SAD) are the main link between ozone chemistry and supersonic aircraft emissions of sulphur precursors (SO2) and particles (H2O-H2SO4). Photochemical O3 changes are compared from four independent 3-D atmosphere-chemistry models (ACMs), using as input the perturbation of SSA-SAD calculated in the University of L'Aquila model, which includes on-line a microphysics code for aerosol formation and growth. The ACMs in this study use aircraft emission scenarios for the year 2050 developed by AIRBUS as a part of the EU project SCENIC, assessing options for fleet size, engine technology (NOx emission index), Mach number, range and cruising altitude. From our baseline modelling simulation, the impact of supersonic aircraft on sulphuric acid aerosol and BC mass burdens is 53 and 1.5 μg/m2, respectively, with a direct RF of −11.4 and 4.6 mW/m2 (net RF=−6.8 mW/m2). This paper discusses the similarities and differences amongst the participating models in terms of O3 precursors changes due to aircraft emissions (NOx, HOx,Clx,Brx) and stratospheric ozone sensitivity to them. In the baseline case, the calculated global ozone change is −0.4±0.3 DU, with a net radiative forcing (IR+UV) of −2.5±2 mW/m2. The fraction of this O3-RF attributable to SSA-SAD changes is, however, highly variable among the models, depending on the NOx removal efficiency from the aircraft emission regions by large scale transport.

Description: The representation of the Tropical Tropopause Layer in 13 different Chemistry Climate Models designed to represent the stratosphere is analyzed. Simulations for 1960–present and 1980–2100 are analyzed and compared to reanalysis model output. Results indicate that the models are able to reproduce the basic structure of the TTL. There is a large spread in cold point tropopause temperatures that may be linked to variation in TTL ozone values. The models are generally able to reproduce historical trends in tropopause pressure obtained from reanalysis products. Simulated historical trends in cold point tropopause temperatures and in the meridional extent of the TTL are not consistent across models. The pressure of both the tropical tropopause and the level of main convective outflow appear to be decreasing (increasing altitude) in historical runs. Similar trends are seen in the future. Models consistently predict decreasing tropopause and convective outflow pressure, by several hPa/decade. Tropical cold point temperatures increase by 0.2 K/decade. This indicates that tropospheric warming dominates stratospheric cooling at the tropical tropopause. Stratospheric water vapor at 100 hPa increases by up to 0.5–1 ppmv by 2100. This is less than implied directly by the temperature and methane increases, highlighting the correlation of tropopause temperatures with stratospheric water vapor, but also the complex nature of TTL transport.

Description: We have estimated impacts of alternative aviation routings on the radiative forcing. Changes in ozone and OH have been estimated in four Chemistry Transport Models (CTMs) participating in the TRADEOFF project. Radiative forcings due to ozone and methane have been calculated accordingly. In addition radiative forcing due to CO2 is estimated based on fuel consumption. Three alternative routing cases are investigated; one scenario assuming additional polar routes and two scenarios assuming aircraft cruising at higher (+2000 ft) and lower (−6000 ft) altitudes. Results from the base case in year 2000 are included as a reference. Taking first a steady state backward looking approach, adding the changes in the forcing from ozone, CO2 and CH4, the ranges of the models used in this work are −0.8 to −1.8 and 0.3 to 0.6 m Wm−2 in the lower (−6000 ft) and higher (+2000 ft) cruise levels, respectively. In relative terms, flying 6000ft lower reduces the forcing by 5–10% compared to the current flight pattern, whereas flying higher, while saving fuel and presumably flying time, increases the forcing by about 2–3%. Taking next a forward looking approach we have estimated the integrated forcing (m Wm−2 yr) over 20 and 100 years time horizons. The relative contributions from each of the three climate gases are somewhat different from the backward looking approach. The differences are moderate adopting 100 year time horizon, whereas under the 20 year horizon CO2 naturally becomes less important relatively. Thus the forcing agents impact climate differently on various time scales. Also, we have found significant differences between the models for ozone and methane. We conclude that we are not yet at a point where we can include non-CO2 effects of aviation in emission trading schemes. Nevertheless, the rerouting cases that have been studied here yield relatively small changes in the radiative forcing due to the radiatively active gases.

Description: Future stratospheric ozone concentrations will be determined both by changes in the concentration of ozone depleting substances (ODSs) and by changes in stratospheric and tropospheric climate, including those caused by changes in anthropogenic greenhouse gases (GHGs). Since future economic development pathways and resultant emissions of GHGs are uncertain, anthropogenic climate change could be a significant source of uncertainty for future projections of stratospheric ozone. In this pilot study, using an "ensemble of opportunity" of chemistry-climate model (CCM) simulations, the contribution of scenario uncertainty from different plausible emissions pathways for ODSs and GHGs to future ozone projections is quantified relative to the contribution from model uncertainty and internal variability of the chemistry-climate system. For both the global, annual mean ozone concentration and for ozone in specific geographical regions, differences between CCMs are the dominant source of uncertainty for the first two-thirds of the 21st century, up-to and after the time when ozone concentrations return to 1980 values. In the last third of the 21st century, dependent upon the set of greenhouse gas scenarios used, scenario uncertainty can be the dominant contributor. This result suggests that investment in chemistry-climate modelling is likely to continue to refine projections of stratospheric ozone and estimates of the return of stratospheric ozone concentrations to pre-1980 levels.

Description: In this work we focus on the direct radiative forcing (RF) of black carbon (BC) and sulphuric acid particles emitted by future supersonic aircraft, as well as on the ozone RF due to changes produced by emissions of both gas species (NOx, H2O) and aerosol particles capable of affecting stratospheric ozone chemistry. Heterogeneous chemical reactions on the surface of sulphuric acid stratospheric particles (SSA-SAD) are the main link between ozone chemistry and supersonic aircraft emissions of sulphur precursors (SO2) and particles (H2O–H2SO4). Photochemical O3 changes are compared from four independent 3-D atmosphere-chemistry models (ACMs), using as input the perturbation of SSA-SAD calculated in the University of L'Aquila model, which includes on-line a microphysics code for aerosol formation and growth. The ACMs in this study use aircraft emission scenarios for the year 2050 developed by AIRBUS as a part of the EU project SCENIC, assessing options for fleet size, engine technology (NOx emission index), Mach number, range and cruising altitude. From our baseline modeling simulation, the impact of supersonic aircraft on sulphuric acid aerosol and BC mass burdens is 53 and 1.5 μg/m2, respectively, with a direct RF of −11.4 and 4.6 mW/m2 (net RF=−6.8 mW/m2). This paper discusses the similarities and differences amongst the participating models in terms of changes to O3 precursors due to aircraft emissions (NOx, HOx,Clx,Brx) and the stratospheric ozone sensitivity to them. In the baseline case, the calculated global ozone change is −0.4 ±0.3 DU, with a net radiative forcing (IR+UV) of −2.5± 2 mW/m2. The fraction of this O3-RF attributable to SSA-SAD changes is, however, highly variable among the models, depending on the NOx removal efficiency from the aircraft emission regions by large scale transport.