The transport sector emits a wide variety of gases and aerosols, with distinctly different characteristics which influence climate directly and indirectly via chemical and physical processes. Tools that allow these emissions to be placed on some kind of common scale in terms of their impact on climate have a number of possible uses such as: in agreements and emission trading schemes; when considering potential trade-offs between changes in emissions resulting from technological or operational developments; and/or for comparing the impact of different environmental impacts of transport activities. Many of the non-CO 2 emissions from the transport sector are short-lived substances, not currently covered by the Kyoto Protocol. There are formidable difficulties in developing metrics and these are particularly acute for such short-lived species. One difficulty concerns the choice of an appropriate structure for the metric (which may depend on, for example, the design of any climate policy it is intended to serve) and the associated value judgements on the appropriate time periods to consider; these choices affect the perception of the relative importance of short-and long-lived species. A second difficulty is the quantification of input parameters (due to underlying uncertainty in atmospheric processes). In addition, for some transport-related emissions, the values of metrics (unlike the gases included in the Kyoto Protocol) depend on where and when the emissions are introduced into the atmosphere-both the regional distribution and, for aircraft, the distribution as a function of altitude, are important. In this assessment of such metrics, we present Global Warming Potentials (GWPs) as these have traditionally been used in the implementation of climate policy. We also present Global Temperature Change Potentials (GTPs) as an alternative metric, as this, or a similar metric may be more appropriate for use in some circumstances. We use radiative forcings and lifetimes from the literature to derive GWPs and GTPs for the main transport-related emissions, and discuss the uncertainties in these estimates. We find large variations in metric (GWP and GTP) values for NO x , mainly due to the dependence on location of emissions but also because of inter-model differences and differences in experimental design. For aerosols we give only global-mean values due to an inconsistent picture amongst available studies regarding regional dependence. The uncertainty in the presented metric values reflects the current state of understanding; the ranking of the various components with respect to our confidence in the given metric values is also given. While the focus is mostly on metrics for comparing the climate impact of emissions, many of the issues are equally relevant for stratospheric ozone depletion metrics, which are also discussed.

Interest in stratospheric aerosol and its role in climate have increased over the last decade due to the observed increase in stratospheric aerosol since 2000 and the potential for changes in the sulfur cycle induced by climate change. This review provides an overview about the advances in stratospheric aerosol research since the last comprehensive assessment of stratospheric aerosol was published in 2006. A crucial development since 2006 is the substantial improvement in the agreement between in situ and space-based inferences of stratospheric aerosol properties during volcanically quiescent periods. Furthermore, new measurement systems and techniques, both in situ and space based, have been developed for measuring physical aerosol properties with greater accuracy and for characterizing aerosol composition. However, these changes induce challenges to constructing a long-term stratospheric aerosol climatology. Currently, changes in stratospheric aerosol levels less than 20% cannot be confidently quantified. The volcanic signals tend to mask any nonvolcanically driven change, making them difficult to understand. While the role of carbonyl sulfide as a substantial and relatively constant source of stratospheric sulfur has been confirmed by new observations and model simulations, large uncertainties remain with respect to the contribution from anthropogenic sulfur dioxide emissions. New evidence has been provided that stratospheric aerosol can also contain small amounts of nonsulfate matter such as black carbon and organics. Chemistry-climate models have substantially increased in quantity and sophistication. In many models the implementation of stratospheric aerosol processes is coupled to radiation and/or stratospheric chemistry modules to account for relevant feedback processes.

Abstract. 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 intermodel 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.

Abstract. Ozone forms in the Earth's atmosphere from the photodissociation of molecular oxygen, primarily in the tropical stratosphere. It is then transported to the extratropics by the Brewer-Dobson circulation (BDC), forming a protective "ozone layer" around the globe. Human emissions of halogen-containing ozone-depleting substances (hODSs) led to a decline in stratospheric ozone until they were banned by the Montreal Protocol, and since 1998 ozone in the upper stratosphere is rising again, likely the recovery from halogeninduced losses. Total column measurements of ozone between the Earth's surface and the top of the atmosphere indicate that the ozone layer has stopped declining across the globe, but no clear increase has been observed at latitudes between 60 • S and 60 • N outside the polar regions (60-90 • ). Here we report evidence from multiple satellite measurements that ozone in the lower stratosphere between 60 • S and 60 • N has indeed continued to decline since 1998. We find that, even though upper stratospheric ozone is recoverPublished by Copernicus Publications on behalf of the European Geosciences Union. 1380 W. T. Ball et al.: Continuous stratospheric ozone decline ing, the continuing downward trend in the lower stratosphere prevails, resulting in a downward trend in stratospheric column ozone between 60 • S and 60 • N. We find that total column ozone between 60 • S and 60 • N appears not to have decreased only because of increases in tropospheric column ozone that compensate for the stratospheric decreases. The reasons for the continued reduction of lower stratospheric ozone are not clear; models do not reproduce these trends, and thus the causes now urgently need to be established.

Wetland methane (CH 4 ) emissions are the largest natural source in the global CH 4 budget, contributing to roughly one third of total natural and anthropogenic emissions. As the second most important anthropogenic greenhouse gas in the atmosphere after CO 2 , CH 4 is strongly associated with climate feedbacks. However, due to the paucity of data, wetland CH 4 feedbacks were not fully assessed in the Intergovernmental Panel on Climate Change Fifth Assessment Report. The degree to which future expansion of wetlands and CH 4 emissions will evolve and consequently drive climate feedbacks is thus a question of major concern. Here we present an ensemble estimate of wetland CH 4 emissions driven by 38 general circulation models for the 21st century. We find that climate changeinduced increases in boreal wetland extent and temperature-driven increases in tropical CH 4 T errestrial wetlands are among the largest biogenic sources of methane contributing to growing atmospheric CH 4 concentrations (1) and are, in turn, highly sensitive to climate change (2). However, radiative feedbacks from wetland CH 4 emissions were not considered in the Coupled Model Intercomparison Project Phase 5 (CMIP5), and Integrated Assessment Models (IAM) assumed anthropogenic sources to be the only driver responsible for the increase of atmospheric CH 4 burden since the 1750s (3). The role of wetland CH 4 emissions, however, may play an increasingly larger role in future atmospheric growth of methane because of the large stocks of mineral and organic carbon stored under anaerobic conditions in both boreal and tropical regions. Paleoclimatological and contemporary observations of the climate sensitivity of wetland methane emissions suggest the potential for a large feedback (4), but there remains large uncertainty in quantifying the actual range of the response (5, 6).Increasing air temperature is linked to the thawing of permafrost and to increased rates of soil microbial activity (7), which directly lead to greater CH 4 production in soils due to thaw-induced change in surface wetland areas (8). In the tropics, wetland areal extent is also influenced by precipitation, which affects the area of surface inundation, water table depth, and soil moisture that, in turn, promote methanogenesis. Elevated CO 2 concentrations can increase ecosystem water use efficiency and thus soil moisture, and also increase soil carbon substrate availability for microbial activities (9). Tropical wetlands, for which a decline in inundation was observed in recent decades (10), are already exposed to increasing frequencies in extreme climate events, e.g., heat waves, floods, and droughts, and changes in rainfall distribution (11) and variability in methane emissions (12). Meanwhile, northern highlatitude ecosystems are experiencing a more rapid temperature increase than elsewhere globally and with increased rates of soil respiration (13), yet, locally at least, no response in methane emissions (14). Despite the importance of these feedbacks noted by the Intergovernmen...

The global atmospheric sulfur budget and its emission dependence have been investigated using the coupled aerosol-chemistry-climate model SOCOL-AER. The aerosol module comprises gaseous and aqueous sulfur chemistry and comprehensive microphysics. The particle distribution is resolved by 40 size bins spanning radii from 0.39 nm to 3.2 μm, including size-dependent particle composition. Aerosol radiative properties required by the climate model are calculated online from the aerosol module. The model successfully reproduces main features of stratospheric aerosols under nonvolcanic conditions, including aerosol extinctions compared to Stratospheric Aerosol and Gas Experiment II (SAGE II) and Halogen Occultation Experiment, and size distributions compared to in situ measurements. The calculated stratospheric aerosol burden is 109 Gg of sulfur, matching the SAGE II-based estimate (112 Gg). In terms of fluxes through the tropopause, the stratospheric aerosol layer is due to about 43% primary tropospheric aerosol, 28% SO 2 , 23% carbonyl sulfide (OCS), 4% H 2 S, and 2% dimethyl sulfide (DMS). Turning off emissions of the short-lived species SO 2 , H 2 S, and DMS shows that OCS alone still establishes about 56% of the original stratospheric aerosol burden. Further sensitivity simulations reveal that anticipated increases in anthropogenic SO 2 emissions in China and India have a larger influence on stratospheric aerosols than the same increase in Western Europe or the U.S., due to deep convection in the western Pacific region. However, even a doubling of Chinese and Indian emissions is predicted to increase the stratospheric background aerosol burden only by 9%. In contrast, small to moderate volcanic eruptions, such as that of Nabro in 2011, may easily double the stratospheric aerosol loading.

Abstract. We present the third generation of the coupled chemistry-climate model (CCM) SOCOL (modeling tools for studies of SOlar Climate Ozone Links). The most notable modifications compared to the previous model version are (1) the dynamical core has been updated with the fifth generation of the middle-atmosphere general circulation model MA-ECHAM (European Centre/HAMburg climate model), and (2) the advection of the chemical species is now calculated by a mass-conserving and shape-preserving flux-form transport scheme instead of the previously used hybrid advection scheme. The whole chemistry code has been rewritten according to the ECHAM5 infrastructure and transferred to Fortran95. In contrast to its predecessors, SOCOLvs3 is now fully parallelized. The performance of the new SOCOL version is evaluated on the basis of transient model simulations (1975-2004) with different horizontal (T31 and T42) resolutions, following the approach of the CCMVal-1 model validation activity. The advanced advection scheme significantly reduces the artificial loss and accumulation of tracer mass in regions with strong gradients that was observed in previous model versions. Compared to its predecessors, SOCOLvs3 generally shows more realistic distributions of chemical trace species, especially of total inorganic chlorine, in terms of the mean state, but also of the annual and interannual variability. Advancements with respect to model dynamics are for example a better representation of the stratospheric mean state in spring, especially in the Southern Hemisphere, and a slowdown of the upward propagation in the tropical lower stratosphere. Despite a large number of improvements model deficiencies still remain. Examples include a too-fast vertical ascent and/or horizontal mixing in the tropical stratosphere, the cold temperature bias in the lowermost polar stratosphere, and the overestimation of polar total ozone loss during Antarctic springtime.

Abstract. 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.