Global warming potentials and radiative efficiencies of halocarbons and related compounds: a comprehensive review

In the mid-1970s it was recognized that, as well as being substances that deplete stratospheric ozone, chlorofluorocarbons (CFCs) were strong greenhouse gases that could have substantial impacts on radiative forcing of climate change. Around a decade later, this group of radiatively active compounds was expanded to include a large number of replacements for ozone-depleting substances such as chlorocarbons, hydrochlorocarbons, hydrochlorofluorocarbons (HCFCs), hydrofluorocarbons (HFCs), perfluorocarbons (PFCs), bromofluorocarbons, and bromochlorofluorocarbons. This paper systematically reviews the published literature concerning the radiative efficiencies (REs) of CFCs, bromofluorocarbons and bromochlorofluorocarbons (halons), HCFCs, HFCs, PFCs, SF6, NF3, and related halogen containing compounds. In addition we provide a comprehensive and self-consistent set of new calculations of REs and global warming potentials (GWPs) for these compounds, mostly employing atmospheric lifetimes taken from the available literature. We also present Global Temperature change Potentials (GTPs) for selected gases. Infrared absorption spectra used in the RE calculations were taken from databases and individual studies, and from experimental and ab initio computational studies. Evaluations of REs and GWPs are presented for more than 200 compounds. Our calculations yield REs significantly (> 5%) different from those in the Intergovernmental Panel on Climate Change Fourth Assessment Report (AR4) for 49 compounds. We present new RE values for more than 100 gases which were not included in AR4. A widely-used simple method to calculate REs and GWPs from absorption spectra and atmospheric lifetimes is assessed and updated. This is the most comprehensive review of the radiative efficiencies and global warming potentials of halogenated compounds performed to date.

Comment on "Tropospheric temperature response to stratospheric ozone recovery in the 21st century" by Hu et al. (2011)

Abstract. In a recent paper Hu et al. (2011) suggest that the recovery of stratospheric ozone during the first half of this century will significantly enhance free tropospheric and surface warming caused by the anthropogenic increase of greenhouse gases, with the effects being most pronounced in Northern Hemisphere middle and high latitudes. These surprising results are based on a multi-model analysis of CMIP3 model simulations with and without prescribed stratospheric ozone recovery. Hu et al. suggest that in order to properly quantify the tropospheric and surface temperature response to stratospheric ozone recovery, it is necessary to run coupled atmosphere-ocean climate models with stratospheric ozone chemistry. The results of such an experiment are presented here, using a state-of-the-art chemistry-climate model coupled to a three-dimensional ocean model. In contrast to Hu et al., we find a much smaller Northern Hemisphere tropospheric temperature response to ozone recovery, which is of opposite sign. We suggest that their result is an artifact of the incomplete removal of the large effect of greenhouse gas warming between the two different sets of models.

Projections of UV radiation changes in the 21st century: impact of ozone recovery and cloud effects

Monthly averaged surface erythemal solar irradiance (UV-Ery) for local noon from 1960 to 2100 has been derived using radiative transfer calculations and projections of ozone, temperature and cloud change from 14 chemistry climate models (CCM), as part of the CCMVal-2 activity of SPARC. Our calculations show the influence of ozone depletion and recovery on erythemal irradiance. In addition, we investigate UV-Ery changes caused by climate change due to increasing greenhouse gas concentrations. The latter include effects of both stratospheric ozone and cloud changes. The derived estimates provide a global picture of the likely changes in erythemal irradiance during the 21st century. Uncertainties arise from the assumed scenarios, different parameterizations – particularly of cloud effects on UV-Ery – and the spread in the CCM projections. The calculations suggest that relative to 1980, annually mean UV-Ery in the 2090s will be on average 12% lower at high latitudes in both hemispheres, 3% lower at mid latitudes, and marginally higher (1 %) in the tropics. The largest reduction (16 %) is projected for Antarctica in October. Cloud effects are responsible for 2–3% of the reduction in UV-Ery at high latitudes, but they slightly moderate it at mid-latitudes (1 %). The year of return of erythemal irradiance to values of certain milestones (1965 and 1980) depends largely on the return of column ozone to the corresponding levels and is associated with large uncertainties mainly due to the spread of the model projections. The inclusion of cloud effects in the calculations has only a small effect of the return years. At mid and high latitudes, changes in clouds and stratospheric ozone transport by global circulation changes due to greenhouse gases will sustain the erythemal irradiance at levels below those in 1965, despite the removal of ozone depleting substances.

Review of the formulation of present‐generation stratospheric chemistry‐climate models and associated external forcings

The goal of the Chemistry‐Climate Model Validation (CCMVal) activity is to improve understanding of chemistry‐climate models (CCMs) through process‐oriented evaluation and to provide reliable projections of stratospheric ozone and its impact on climate. An appreciation of the details of model formulations is essential for understanding how models respond to the changing external forcings of greenhouse gases and ozonedepleting substances, and hence for understanding the ozone and climate forecasts produced by the models participating in this activity. Here we introduce and review the models used for the second round (CCMVal‐2) of this intercomparison, regarding the implementation of chemical, transport, radiative, and dynamical processes in these models. In particular, we review the advantages and problems associated with approaches used to model processes of relevance to stratospheric dynamics and chemistry. Furthermore, we state the definitions of the reference simulations performed, and describe the forcing data used in these simulations. We identify some developments in chemistry‐climate modeling that make models more physically based or more comprehensive, including the introduction of an interactive ocean, online photolysis, troposphere‐stratosphere chemistry, and non‐orographic gravity‐wave deposition as linked to tropospheric convection. The relatively new developments indicate that stratospheric CCM modeling is becoming more consistent with our physically based understanding of the atmosphere.

Separating the dynamical effects of climate change and ozone depletion. Part I: Southern Hemisphere stratosphere

A version of the Canadian Middle Atmosphere Model that is coupled to an ocean is used to investigate the separate effects of climate change and ozone depletion on the dynamics of the Southern Hemisphere (SH) stratosphere. This is achieved by performing three sets of simulations extending from 1960 to 2099: 1) greenhouse gases (GHGs) fixed at 1960 levels and ozone depleting substances (ODSs) varying in time, 2) ODSs fixed at 1960 levels and GHGs varying in time, and 3) both GHGs and ODSs varying in time. The response of various dynamical quantities to theGHGand ODS forcings is shown to be additive; that is, trends computed from the sum of the first two simulations are equal to trends from the third. Additivity is shown to hold for the zonal mean zonal wind and temperature, the mass flux into and out of the stratosphere, and the latitudinally averaged wave drag in SH spring and summer, as well as for final warming dates. Ozone depletion and recovery causes seasonal changes in lower-stratosphere mass flux, with reduced polar downwelling in the past followed by increased downwelling in the future in SH spring, and the reverse in SH summer. These seasonal changes are attributed to changes in wave drag caused by ozone-induced changes in the zonal mean zonal winds. Climate change, on the other hand, causes a steady decrease in wave drag during SH spring, which delays the breakdown of the vortex, resulting in increased wave drag in summer

Chemistry–climate model simulations of twenty-first century stratospheric climate and circulation changes

The response of stratospheric climate and circulation to increasing amounts of greenhouse gases (GHGs) and ozone recovery in the twenty-first century is analyzed in simulations of 11 chemistry–climate models using near-identical forcings and experimental setup. In addition to an overall global cooling of the stratosphere in the simulations (0.59 6 0.07 K decade21 at 10 hPa), ozone recovery causes a warming of the Southern Hemisphere polar lower stratosphere in summer with enhanced cooling above. The rate of warming correlates with the rate of ozone recovery projected by the models and, on average, changes from 0.8 to 0.48 Kdecade21 at 100 hPa as the rate of recovery declines from the first to the second half of the century. In the winter northern polar lower stratosphere the increased radiative cooling from the growing abundance of GHGs is, in most models, balanced by adiabatic warming from stronger polar downwelling. In the Antarctic lower stratosphere the models simulate an increase in low temperature extremes required for polar stratospheric cloud (PSC) formation, but the positive trend is decreasing over the twenty-first century in all models. In the Arctic, none of the models simulates a statistically significant increase in Arctic PSCs throughout the twenty-first century. The subtropical jets accelerate in response to climate change and the ozone recovery produces awestward acceleration of the lower-stratosphericwind over theAntarctic during summer, though this response is sensitive to the rate of recovery projected by the models. There is a strengthening of the Brewer–Dobson circulation throughout the depth of the stratosphere, which reduces the mean age of air nearly everywhere at a rate of about 0.05 yr decade21 in those models with this diagnostic. On average, the annual mean tropical upwelling in the lower stratosphere (;70 hPa) increases by almost 2% decade21, with 59% of this trend forced by the parameterized orographic gravity wave drag in the models. This is a consequence of the eastward acceleration of the subtropical jets, which increases the upward flux of (parameterized) momentum reaching the lower stratosphere in these latitudes.

What is the climate system able to do ‘on its own’?

The climate of the Earth, like planetary climates in general, is broadly controlled by solar irradiation, planetary albedo and emissivity as well as its rotation rate and distribution of land (with its orography) and oceans. However, the majority of climate fluctuations that affect mankind are internal modes of the general circulation of the atmosphere and the oceans. Some of these modes, such as El Nino-Southern Oscillation (ENSO), are quasi-regular and have some longer-term predictive skill; others like the Arctic and Antarctic Oscillation are chaotic and generally unpredictable beyond a few weeks. Studies using general circulation models indicate that internal processes dominate the regional climate and that some like ENSO events have even distinct global signatures. This is one of the reasons why it is so difficult to separate internal climate processes from external ones caused, for example, by changes in greenhouse gases and solar irradiation. However, the accumulation of the warmest seasons during the latest two decades is lending strong support to the forcing of the greenhouse gases. As models are getting more comprehensive, they show a gradually broader range of internal processes including those on longer time scales, challenging the interpretation of the causes of past and present climate events further.

Geo-Engineering to Confine Climate Change: Is it at all Feasible?

Paul Crutzen (2006) has suggested a research initiative to consider whether it would be feasible to artificially enhance the albedo of the planet Earth to counteract greenhouse warming. The enhancement of albedo would be achieved by intentionally injecting sulfur into the stratosphere. The rational for proposing the experiment is the observed cooling of the atmosphere following the recent major volcanic eruptions by El Chichon in 1984 and Mount Pinatubo in 1991 (Hansen et al., 1992). Although I am principally not against a research initiative to study such a potential experiment, I do have important reservations concerning its general feasibility. And its potential feasibility, I believe, must be the key motivation for embarking on such a study. Here I will bring up three major issues, which must be more thoroughly understood before any geo-engineering of climate could be considered, if at all. The three issues are (i) the lack of accuracy in climate prediction, (ii) the huge difference in timescale between the effect of greenhouse gases and the effect of aerosols and (iii) serious environmental problems which may be caused by high carbon dioxide concentration irrespective of the warming of the climate.

Origin of regional climate differences: role of boundary conditions and model formulation in two GCMs

Model differences in projections of extratropical regional climate change due to increasing greenhouse gases are investigated using two atmospheric general circulation models (AGCMs): ECHAM4 (Max Planck Institute, version 4) and CCM3 (National Center for Atmospheric Research Community Climate Model version 3). Sea-surface temperature (SST) fields calculated from observations and coupled versions of the two models are used to force each AGCM in experiments based on time-slice methodology. Results from the forced AGCMs are then compared to coupled model results from the Coupled Model Intercomparison Project 2 (CMIP2) database. The time-slice methodology is verified by showing that the response of each model to doubled CO2 and SST forcing from the CMIP2 experiments is consistent with the results of the coupled GCMs. The differences in the responses of the models are attributed to (1) the different tropical SST warmings in the coupled simulations and (2) the different atmospheric model responses to the same tropical SST warmings. Both are found to have important contributions to differences in implied Northern Hemisphere (NH) winter extratropical regional 500 mb height and tropical precipitation climate changes. Forced teleconnection patterns from tropical SST differences are primarily responsible for sensitivity differences in the extratropical North Pacific, but have relatively little impact on the North Atlantic. There are also significant differences in the extratropical response of the models to the same tropical SST anomalies due to differences in numerical and physical parameterizations. Differences due to parameterizations dominate in the North Atlantic. Differences in the control climates of the two coupled models from the current climate, in particular for the coupled model containing CCM3, are also demonstrated to be important in leading to differences in extratropical regional sensitivity.

Why is the global warming proceeding much slower than expected?

Upper air observations from radiosondes and microwave satellite instruments does not indicate any global warming during the last 19 years, contrary to surface measurements, where a warming trend is supposedly being found. This result is somewhat difficult to reconcile, since climate model experiments do indicate a reverse trend, namely, that upper tropospheric air should warm faster than the surface. To contribute toward an understanding of this difficulty, we have here undertaken some specific experiments to study the effect on climate due to the decrease in stratospheric ozone and the Mount Pinatubo eruption in 1991. The associated forcing was added to the forcing from greenhouse gases, sulfate aerosols (direct and indirect effect), and tropospheric ozone, which was investigated in a separate series of experiments. Furthermore, we have undertaken an ensemble study in order to explore the natural variability of an advanced climate model exposed to such a forcing over 19 years. The result shows that the reduction of stratospheric ozone cools not only the lower stratosphere but also the troposphere, in particular, the upper and middle part. In the upper troposphere the cooling from stratospheric ozone leads to a significant reduction of greenhouse warming. The modeled stratospheric aerosols from Mount Pinatubo generate a climate response (stratospheric warming and tropospheric cooling) in good agreement with microwave satellite measurements. Finally, analysis of a series of experiments with both stratospheric ozone and the Mount Pinatubo effect shows considerable variability in climate response, suggesting that an evolution having no warming in the period is as likely as another evolution showing modest warming. However, the observed trend of no warming in the midtroposphere and clear warming at the surface is not found in the model simulations.

Transient climate change simulations with a coupled atmosphere–ocean GCM including the tropospheric sulfur cycle

The time-dependent climate response to changing concentrations of greenhouse gases and sulfate aerosols is studied using a coupled general circulation model of the atmosphere and the ocean (ECHAM4/OPYC3). The concentrations of the well-mixed greenhouse gases like CO2, CH4, N2O, and CFCs are prescribed for the past (1860–1990) and projected into the future according to International Panel on Climate Change (IPCC) scenario IS92a. In addition, the space–time distribution of tropospheric ozone is prescribed, and the tropospheric sulfur cycle is calculated within the coupled model using sulfur emissions of the past and projected into the future (IS92a). The radiative impact of the aerosols is considered via both the direct and the indirect (i.e., through cloud albedo) effect. It is shown that the simulated trend in sulfate deposition since the end of the last century is broadly consistent with ice core measurements, and the calculated radiative forcings from preindustrial to present time are within the uncertainty range estimated by IPCC. Three climate perturbation experiments are performed, applying different forcing mechanisms, and the results are compared with those obtained from a 300-yr unforced control experiment. As in previous experiments, the climate response is similar, but weaker, if aerosol effects are included in addition to greenhouse gases. One notable difference to previous experiments is that the strength of the Indian summer monsoon is not fundamentally affected by the inclusion of aerosol effects. Although the monsoon is damped compared to a greenhouse gas only experiment, it is still more vigorous than in the control experiment. This different behavior, compared to previous studies, is the result of the different land–sea distribution of aerosol forcing. Somewhat unexpected, the intensity of the global hydrological cycle becomes weaker in a warmer climate if both direct and indirect aerosol effects are included in addition to the greenhouse gases. This can be related to anomalous net radiative cooling of the earth’s surface through aerosols, which is balanced by reduced turbulent transfer of both sensible and latent heat from the surface to the atmosphere.

Impact of global warming on the interannual and interdecadal climate modes in a coupled GCM

In this study, we investigated the impact of global warming on the variabilities of large-scale interannual and interdecadal climate modes and teleconnection patterns with two long-term integrations of the coupled general circulation model of ECHAM4/OPYC3 at the Max-Planck-Institute for Meteorology, Hamburg. One is the control (CTRL) run with fixed present-day concentrations of greenhouse gases. The other experiment is a simulation of transient greenhouse warming, named GHG run. In the GHG run the averaged geopotential height at 500 hPa is increased significantly, and a negative phase of the Pacific/North American (PNA) teleconnection-like distribution pattern is intensified. The standard deviation over the tropics (high latitudes) is enhanced (reduced) on the interdecadal time scales and reduced (enhanced) on the interannual time scales in the GHG run. Except for an interdecadal mode related to the Southern Oscillation (SO) in the GHG run, the spatial variation patterns are similar for different (interannual + interdecadal, interannual, and interdecadal) time scales in the GHG and CTRL runs. Spatial distributions of the teleconnection patterns on the interannual and interdecadal time scales in the GHG run are also similar to those in the CTRL run. But some teleconnection patterns show linear trends and changes of variances and frequencies in the GHG run. Apart from the positive linear trend of the SO, the interdecadal modulation to the El Niño/SO cycle is enhanced during the GHG 2040 ∼ 2099. This is the result of an enhancement of the Walker circulation during that period. La Niña events intensify and El Niño events relatively weaken during the GHG 2070 ∼ 2090. It is interesting to note that with increasing greenhouse gas concentrations the relation between the SO and the PNA pattern is reversed significantly from a negative to a positive correlation on the interdecadal time scales and weakened on the interannual time scales. This suggests that the increase of the greenhouse gas concentrations will trigger the nonstationary correlation between the SO and the PNA pattern both on the interdecadal and interannual time scales.

The effect of nonlinearity in CO2 heating rates on the attribution of stratospheric ozone and temperature changes

An analysis of the attribution of past and future changes in stratospheric ozone and temperature to anthropogenic forcings is presented. The analysis is an extension of the study of Shepherd and Jonsson (2008) who analyzed chemistry-climate simulations from the Canadian Middle Atmosphere Model (CMAM) and attributed both past and future changes to changes in the external forcings, i.e. the abundances of ozone-depleting substances (ODS) and well-mixed greenhouse gases. The current study is based on a new CMAM dataset and includes two important changes. First, we account for the nonlinear radiative response to changes in CO2. It is shown that over centennial time scales the radiative response in the upper stratosphere to CO2 changes is significantly nonlinear and that failure to account for this effect leads to a significant error in the attribution. To our knowledge this nonlinearity has not been considered before in attribution analysis, including multiple linear regression studies. For the regression analysis presented here the nonlinearity was taken into account by using CO2 heating rate, rather than CO2 abundance, as the explanatory variable. This approach yields considerable corrections to the results of the previous study and can be recommended to other researchers. Second, an error in the way the CO2 forcing changes are implemented in the CMAM was corrected, which significantly affects the results for the recent past. As the radiation scheme, based on Fomichev et al. (1998), is used in several other models we provide some description of the problem and how it was fixed.

Dynamics, stratospheric ozone, and climate change

Dynamics affects the distribution and abundance of stratospheric ozone directly through transport of ozone itself and indirectly through its effect on ozone chemistry via temperature and transport of other chemical species. Dynamical processes must be considered in order to understand past ozone changes, especially in the northern hemisphere where there appears to be significant low-frequency variability which can look “trend-like” on decadal time scales. A major challenge is to quantify the predictable, or deterministic, component of past ozone changes. Over the coming century, changes in climate will affect the expected recovery of ozone. For policy reasons it is important to be able to distinguish and separately attribute the effects of ozone-depleting substances and greenhouse gases on both ozone and climate. While the radiative-chemical effects can be relatively easily identified, this is not so evident for dynamics — yet dynamical changes (e.g., changes in the Brewer-Dobson circulation) could have a first-order effect on ozone over particular regions. Understanding the predictability and robustness of such dynamical changes represents another major challenge. Chemistry-climate models have recently emerged as useful tools for addressing these questions, as they provide a self-consistent representation of dynamical aspects of climate and their coupling to ozone chemistry. We can expect such models to play an increasingly central role in the study of ozone and climate in the future, analogous to the central role of global climate models in the study of tropospheric climate change.

Multimodel projections of stratospheric ozone in the 21st century

Simulations from eleven coupled chemistry-climate models (CCMs) employing nearly identical forcings have been used to project the evolution of stratospheric ozone throughout the 21st century. The model-to-model agreement in projected temperature trends is good, and all CCMs predict continued, global mean cooling of the stratosphere over the next 5 decades, increasing from around 0.25 K/decade at 50 hPa to around 1 K/ decade at 1 hPa under the Intergovernmental Panel on Climate Change (IPCC) Special Report on Emissions Scenarios (SRES) A1B scenario. In general, the simulated ozone evolution is mainly determined by decreases in halogen concentrations and continued cooling of the global stratosphere due to increases in greenhouse gases (GHGs). Column ozone is projected to increase as stratospheric halogen concentrations return to 1980s levels. Because of ozone increases in the middle and upper stratosphere due to GHGinduced cooling, total ozone averaged over midlatitudes, outside the polar regions, and globally, is projected to increase to 1980 values between 2035 and 2050 and before lower stratospheric halogen amounts decrease to 1980 values. In the polar regions the CCMs simulate small temperature trends in the first and second half of the 21st century in midwinter. Differences in stratospheric inorganic chlorine (Cly) among the CCMs are key to diagnosing the intermodel differences in simulated ozone recovery, in particular in the Antarctic. It is found that there are substantial quantitative differences in the simulated Cly, with the October mean Antarctic Cly peak value varying from less than 2 ppb to over 3.5 ppb in the CCMs, and the date at which the Cly returns to 1980 values varying from before 2030 to after 2050. There is a similar variation in the timing of recovery of Antarctic springtime column ozone back to 1980 values. As most models underestimate peak Cly near 2000, ozone recovery in the Antarctic could occur even later, between 2060 and 2070. In the Arctic the column ozone increase in spring does not follow halogen decreases as closely as in the Antarctic, reaching 1980 values before Arctic halogen amounts decrease to 1980 values and before the Antarctic. None of the CCMs predict future large decreases in the Arctic column ozone. By 2100, total column ozone is projected to be substantially above 1980 values in all regions except in the tropics.