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This paper draws from the experience of the 3-year, Horizon 2020 project, AI4PublicPolicy, and examines the essential actions public municipalities should take to adequately prepare for the integration of Artificial Intelligence (AI) into their policy making processes under the scope of the five pilot cities involved in the project. The study explores a range of issues including organisational, technological, and ethical aspects. It also underlines the importance to understand local environments, involve stakeholders, evaluate the relevance and the availability of the data, assess the technological readiness, improve internal capacities and assure legal and ethical compliance. In order to promote transparency and cultivate public trust, the document also emphasizes the significance of elaborating on user-centric, agile and stable AI-based tools and solutions, such as dashboards of Explainable AI (XAI) services. Municipalities may pave their way towards automated, transparent and citizen-centric development of public policies by handling the challenges of AI deployment with the help of the current framework.

Fire is an integral ecosystem process and a major natural source of vegetation disturbance globally. Yet at the same time, humans use and manage fire in diverse ways and for a huge range of purposes. Therefore, it is perhaps unsurprising that a central finding of the first Fire Model Intercomparison Project was simplistic representation of humans is a substantial shortcoming in the fire modules of dynamic global vegetation models (DGVMs). In response to this challenge, we present a novel, global geospatial model that seeks to capture the diversity of human–fire interactions. Empirically grounded with a global database of anthropogenic fire impacts, WHAM! (the Wildfire Human Agency Model) represents the underlying behavioural and land system drivers of human approaches to fire management and their impact on fire regimes. WHAM! is designed to be coupled with DGVMs (JULES-INFERNO in the current instance), such that human and biophysical drivers of fire on Earth, and their interactions, can be captured in process-based models for the first time. Initial outputs from WHAM! presented here are in line with previous evidence suggesting managed anthropogenic fire use is decreasing globally and point to land use intensification as the underlying reason for this phenomenon.

Peat fires in the northern high latitudes have the potential to burn vast amounts of carbon-rich organic soil, releasing large quantities of long-term stored carbon to the atmosphere. Due to anthropogenic activities and climate change, peat fires are increasing in frequency and intensity across the high latitudes. However, at present they are not explicitly included in most fire models. Here we detail the development of INFERNO-peat, the first parameterization of peat fires in the JULES-INFERNO (Joint UK Land Environment Simulator INteractive Fire and Emission algoRithm for Natural envirOnments) fire model. INFERNO-peat utilizes knowledge from lab and field-based studies on peat fire ignition and spread to be able to model peat burnt area, burn depth, and carbon emissions, based on data of the moisture content, inorganic content, bulk density, soil temperature, and water table depth of peat. INFERNO-peat improves the representation of burnt area in the high latitudes, with peat fires simulating on average an additional 0.305×106 km2 of burn area each year, emitting 224.10 Tg of carbon. Compared to Global Fire Emissions Database version 5 (GFED5), INFERNO-peat captures ∼ 20 % more burnt area, whereas INFERNO underestimated burning by 50 %. Additionally, INFERNO-peat substantially improves the representation of interannual variability in burnt area and subsequent carbon emissions across the high latitudes. The coefficient of variation in carbon emissions is increased from 0.071 in INFERNO to 0.127 in INFERNO-peat, an almost 80 % increase. Therefore, explicitly modelling peat fires shows a substantial improvement in the fire modelling capabilities of JULES-INFERNO, highlighting the importance of representing peatland systems in fire models.

The climate science community aims to improve our understanding of climate change due to anthropogenic influences on atmospheric composition and the Earth's surface. Yet not all climate interactions are fully understood, and uncertainty in climate model results persists, as assessed in the latest Intergovernmental Panel on Climate Change (IPCC) assessment report. We synthesize current challenges and emphasize opportunities for advancing our understanding of the interactions between atmospheric composition, air quality, and climate change, as well as for quantifying model diversity. Our perspective is based on expert views from three multi-model intercomparison projects (MIPs) – the Precipitation Driver Response MIP (PDRMIP), the Aerosol Chemistry MIP (AerChemMIP), and the Radiative Forcing MIP (RFMIP). While there are many shared interests and specializations across the MIPs, they have their own scientific foci and specific approaches. The partial overlap between the MIPs proved useful for advancing the understanding of the perturbation–response paradigm through multi-model ensembles of Earth system models of varying complexity. We discuss the challenges of gaining insights from Earth system models that face computational and process representation limits and provide guidance from our lessons learned. Promising ideas to overcome some long-standing challenges in the near future are kilometer-scale experiments to better simulate circulation-dependent processes where it is possible and machine learning approaches where they are needed, e.g., for faster and better subgrid-scale parameterizations and pattern recognition in big data. New model constraints can arise from augmented observational products that leverage multiple datasets with machine learning approaches. Future MIPs can develop smart experiment protocols that strive towards an optimal trade-off between the resolution, complexity, and number of simulations and their length and, thereby, help to advance the understanding of climate change and its impacts.

Future African aerosol emissions, and therefore air pollution levels and health outcomes, are uncertain and understudied. Understanding the future health impacts of pollutant emissions from this region is crucial. Here, this research gap is addressed by studying the range in the future health impacts of aerosol emissions from Africa in the Shared Socioeconomic Pathway (SSP) scenarios, using the UK Earth System Model version 1 (UKESM1), along with human health concentration–response functions. The effects of Africa following a high-pollution aerosol pathway are studied relative to a low-pollution control, with experiments varying aerosol emissions from industry and biomass burning. Using present-day demographics, annual deaths within Africa attributable to ambient particulate matter are estimated to be lower by 150 000 (5th–95th confidence interval of 67 000–234 000) under stronger African aerosol mitigation by 2090, while those attributable to O3 are lower by 15 000 (5th–95th confidence interval of 9000–21 000). The particulate matter health benefits are realised predominantly within Africa, with the O3-driven benefits being more widespread – though still concentrated in Africa – due to the longer atmospheric lifetime of O3. These results demonstrate the important health co-benefits from future emission mitigation in Africa.

The potential future trend in African aerosol emissions is uncertain, with a large range found in future scenarios used to drive climate projections. The future climate impact of these emissions is therefore uncertain. Using the Shared Socioeconomic Pathway (SSP) scenarios, transient future experiments were performed with the UK Earth System Model (UKESM1) to investigate the effect of African emissions following the high emission SSP370 scenario as the rest of the world follows the more sustainable SSP119, relative to a global SSP119 control. This isolates the effect of Africa following a relatively more polluted future emissions pathway. Compared to SSP119, SSP370 projects higher non-biomass-burning (non-BB) aerosol emissions, but lower biomass burning emissions, over Africa. Increased shortwave (SW) absorption by black carbon aerosol leads to a global warming, but the reduction in the local incident surface radiation close to the emissions is larger, causing a local cooling effect. The local cooling persists even when including the higher African CO2 emissions under SSP370 than SSP119. The global warming is significantly higher by 0.07 K when including the non-BB aerosol increases and higher still (0.22 K) when including all aerosols and CO2. Precipitation also exhibits complex changes. Northward shifts in the Inter-tropical Convergence Zone (ITCZ) occur under relatively warm Northern Hemisphere land, and local rainfall is enhanced due to mid-tropospheric instability from black carbon absorption. These results highlight the importance of future African aerosol emissions for regional and global climate and the spatial complexity of this climate influence.

Fire constitutes a key process in the Earth system (ES), being driven by climate as well as affecting the climate by changing atmospheric composition and impacting the terrestrial carbon cycle. However, studies on the effects of fires on atmospheric composition, radiative forcing and climate have been limited to date, as the current generation of ES models (ESMs) does not include fully atmosphere–composition–vegetation coupled fires feedbacks. The aim of this work is to develop and evaluate a fully coupled fire–composition–climate ES model. For this, the INteractive Fires and Emissions algoRithm for Natural envirOnments (INFERNO) fire model is coupled to the atmosphere-only configuration of the UK's Earth System Model (UKESM1). This fire–atmosphere interaction through atmospheric chemistry and aerosols allows for fire emissions to influence radiation, clouds and generally weather, which can consequently influence the meteorological drivers of fire. Additionally, INFERNO is updated based on recent developments in the literature to improve the representation of human and/or economic factors in the anthropogenic ignition and suppression of fire. This work presents an assessment of the effects of interactive fire coupling on atmospheric composition and climate compared to the standard UKESM1 configuration that uses prescribed fire emissions. Results show a similar performance when using the fire–atmosphere coupling (the “online” version of the model) when compared to the offline UKESM1 that uses prescribed fire. The model can reproduce observed present-day global fire emissions of carbon monoxide (CO) and aerosols, despite underestimating the global average burnt area. However, at a regional scale, there is an overestimation of fire emissions over Africa due to the misrepresentation of the underlying vegetation types and an underestimation over equatorial Asia due to a lack of representation of peat fires. Despite this, comparing model results with observations of CO column mixing ratio and aerosol optical depth (AOD) show that the fire–atmosphere coupled configuration has a similar performance when compared to UKESM1. In fact, including the interactive biomass burning emissions improves the interannual CO atmospheric column variability and consequently its seasonality over the main biomass burning regions – Africa and South America. Similarly, for aerosols, the AOD results broadly agree with the Moderate Resolution Imaging Spectroradiometer (MODIS) and the Aerosol Robotic Network (AERONET) observations.

For the radiative impact of individual climate forcings, most previous studies focused on the global mean values at the top of the atmosphere (TOA), and less attention has been paid to surface processes, especially for black carbon (BC) aerosols. In this study, the surface radiative responses to five different forcing agents were analyzed by using idealized model simulations. Our analyses reveal that for greenhouse gases, solar irradiance, and scattering aerosols, the surface temperature changes are mainly dictated by the changes of surface radiative heating, but for BC, surface energy redistribution between different components plays a more crucial role. Globally, when a unit BC forcing is imposed at TOA, the net shortwave radiation at the surface decreases by -5.87±0.67 W m−2 (W m−2)−1 (averaged over global land without Antarctica), which is partially offset by increased downward longwave radiation (2.32±0.38 W m−2 (W m−2)−1 from the warmer atmosphere, causing a net decrease in the incoming downward surface radiation of -3.56±0.60 W m−2 (W m−2)−1. Despite a reduction in the downward radiation energy, the surface air temperature still increases by 0.25±0.08 K because of less efficient energy dissipation, manifested by reduced surface sensible (-2.88±0.43 W m−2 (W m−2)−1) and latent heat flux (-1.54±0.27 W m−2 (W m−2)−1), as well as a decrease in Bowen ratio (-0.20±0.07 (W m−2)−1). Such reductions of turbulent fluxes can be largely explained by enhanced air stability (0.07±0.02 K (W m−2)−1), measured as the difference of the potential temperature between 925 hPa and surface, and reduced surface wind speed (-0.05±0.01 m s−1 (W m−2)−1). The enhanced stability is due to the faster atmospheric warming relative to the surface, whereas the reduced wind speed can be partially explained by enhanced stability and reduced Equator-to-pole atmospheric temperature gradient. These rapid adjustments under BC forcing occur in the lower atmosphere and propagate downward to influence the surface energy redistribution and thus surface temperature response, which is not observed under greenhouse gases or scattering aerosols. Our study provides new insights into the impact of absorbing aerosols on surface energy balance and surface temperature response.

Atmospheric blocking events are mid-latitude weather patterns, which obstruct the usual path of the polar jet streams. They are often associated with heat waves in summer and cold snaps in winter. Despite being central features of mid-latitude synoptic-scale weather, there is no well-defined historical dataset of blocking events. Various blocking indices (BIs) have thus been suggested for automatically identifying blocking events in observational and in climate model data. However, BIs show significant regional and seasonal differences so that several indices are typically applied in combination to ensure scientific robustness. Here, we introduce a new BI using self-organizing maps (SOMs), an unsupervised machine learning approach, and compare its detection skill to some of the most widely applied BIs. To enable this intercomparison, we first create a new ground truth time series classification of European blocking based on expert judgement. We then demonstrate that our method (SOM-BI) has several key advantages over previous BIs because it exploits all of the spatial information provided in the input data and reduces the dependence on arbitrary thresholds. Using ERA5 reanalysis data (1979–2019), we find that the SOM-BI identifies blocking events with a higher precision and recall than other BIs. In particular, SOM-BI already performs well using only around 20 years of training data so that observational records are long enough to train our new method. We present case studies of the 2003 and 2019 European heat waves and highlight that well-defined groups of SOM nodes can be an effective tool to diagnose such weather events, although the domain-based approach can still lead to errors in the identification of certain events in a fashion similar to the other BIs. We further test the red blocking detection skill of SOM-BI depending on the meteorological variable used to study blocking, including geopotential height, sea level pressure and four variables related to potential vorticity, and the 500 hPa geopotential height anomaly field provides the best results with our new approach. We also demonstrate how SOM-BI can be used to identify different types of blocking events and their associated trends. Finally, we evaluate the SOM-BI performance on around 100 years of climate model data from a pre-industrial simulation with the new UK Earth System Model (UKESM1-0-LL). For the model data, all blocking detection methods have lower skill than for the ERA5 reanalysis, but SOM-BI performs noticeably better than the conventional indices. Overall, our results demonstrate the significant potential for unsupervised learning to complement the study of blocking events in both reanalysis and climate modelling contexts.

The seasonal and longer-term dynamics of fuel accumulation affect fire seasonality and the occurrence of extreme wildfires. Failure to account for their influence may help to explain why state-of-the-art fire models do not simulate the length and timing of the fire season or interannual variability in burnt area well. We investigated the impact of accounting for different timescales of fuel production and accumulation on burnt area using a suite of random forest regression models that included the immediate impact of climate, vegetation, and human influences in a given month and tested the impact of various combinations of antecedent conditions in four productivity-related vegetation indices and in antecedent moisture conditions. Analyses were conducted for the period from 2010 to 2015 inclusive. Inclusion of antecedent vegetation conditions representing fuel build-up led to an improvement of the global, climatological out-of-sample R2 from 0.579 to 0.701, but the inclusion of antecedent vegetation conditions on timescales ≥ 1 year had no impact on simulated burnt area. Current moisture levels were the dominant influence on fuel drying. Additionally, antecedent moisture levels were important for fuel build-up. The models also enabled the visualisation of interactions between variables, such as the importance of antecedent productivity coupled with instantaneous drying. The length of the period which needs to be considered varies across biomes; fuel-limited regions are sensitive to antecedent conditions that determine fuel build-up over longer time periods (∼ 4 months), while moisture-limited regions are more sensitive to current conditions that regulate fuel drying.

Interactions between aerosols and gases in the atmosphere have been the focus of an increasing number of studies in recent years. Here, we focus on aerosol effects on tropospheric ozone that involve meteorological feedbacks induced by aerosol–radiation interactions. Specifically, we study the effects that involve aerosol influences on the transport of gaseous pollutants and on atmospheric moisture, both of which can impact ozone chemistry. For this purpose, we use the UK Earth System Model (UKESM1), with which we performed sensitivity simulations including and excluding the aerosol direct radiative effect (ADE) on atmospheric chemistry, and focused our analysis on an area with a high aerosol presence, namely China. By comparing the simulations, we found that ADE reduced shortwave radiation by 11 % in China and consequently led to lower turbulent kinetic energy, weaker horizontal winds and a shallower boundary layer (with a maximum of 102.28 m reduction in north China). On the one hand, the suppressed boundary layer limited the export and diffusion of pollutants and increased the concentration of CO, SO2, NO, NO2, PM2.5 and PM10 in the aerosol-rich regions. The NO/NO2 ratio generally increased and led to more ozone depletion. On the other hand, the boundary layer top acted as a barrier that trapped moisture at lower altitudes and reduced the moisture at higher altitudes (the specific humidity was reduced by 1.69 % at 1493 m on average in China). Due to reduced water vapour, fewer clouds were formed and more sunlight reached the surface, so the photolytical production of ozone increased. Under the combined effect of the two meteorology feedback methods, the annual average ozone concentration in China declined by 2.01 ppb (6.2 %), which was found to bring the model into closer agreement with surface ozone measurements from different parts of China.

Understanding and quantifying the global methane (CH4) budget is important for assessing realistic pathways to mitigate climate change. Atmospheric emissions and concentrations of CH4 continue to increase, making CH4 the second most important human-influenced greenhouse gas in terms of climate forcing, after carbon dioxide (CO2). The relative importance of CH4 compared to CO2 depends on its shorter atmospheric lifetime, stronger warming potential, and variations in atmospheric growth rate over the past decade, the causes of which are still debated. Two major challenges in reducing uncertainties in the atmospheric growth rate arise from the variety of geographically overlapping CH4 sources and from the destruction of CH4 by short-lived hydroxyl radicals (OH). To address these challenges, we have established a consortium of multidisciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate new research aimed at improving and regularly updating the global methane budget. Following Saunois et al. (2016), we present here the second version of the living review paper dedicated to the decadal methane budget, integrating results of top-down studies (atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up estimates (including process-based models for estimating land surface emissions and atmospheric chemistry, inventories of anthropogenic emissions, and data-driven extrapolations). For the 2008–2017 decade, global methane emissions are estimated by atmospheric inversions (a top-down approach) to be 576 Tg CH4 yr−1 (range 550–594, corresponding to the minimum and maximum estimates of the model ensemble). Of this total, 359 Tg CH4 yr−1 or ∼ 60 % is attributed to anthropogenic sources, that is emissions caused by direct human activity (i.e. anthropogenic emissions; range 336–376 Tg CH4 yr−1 or 50 %–65 %). The mean annual total emission for the new decade (2008–2017) is 29 Tg CH4 yr−1 larger than our estimate for the previous decade (2000–2009), and 24 Tg CH4 yr−1 larger than the one reported in the previous budget for 2003–2012 (Saunois et al., 2016). Since 2012, global CH4 emissions have been tracking the warmest scenarios assessed by the Intergovernmental Panel on Climate Change. Bottom-up methods suggest almost 30 % larger global emissions (737 Tg CH4 yr−1, range 594–881) than top-down inversion methods. Indeed, bottom-up estimates for natural sources such as natural wetlands, other inland water systems, and geological sources are higher than top-down estimates. The atmospheric constraints on the top-down budget suggest that at least some of these bottom-up emissions are overestimated. The latitudinal distribution of atmospheric observation-based emissions indicates a predominance of tropical emissions (∼ 65 % of the global budget, < 30∘ N) compared to mid-latitudes (∼ 30 %, 30–60∘ N) and high northern latitudes (∼ 4 %, 60–90∘ N). The most important source of uncertainty in the methane budget is attributable to natural emissions, especially those from wetlands and other inland waters. Some of our global source estimates are smaller than those in previously published budgets (Saunois et al., 2016; Kirschke et al., 2013). In particular wetland emissions are about 35 Tg CH4 yr−1 lower due to improved partition wetlands and other inland waters. Emissions from geological sources and wild animals are also found to be smaller by 7 Tg CH4 yr−1 by 8 Tg CH4 yr−1, respectively. However, the overall discrepancy between bottom-up and top-down estimates has been reduced by only 5 % compared to Saunois et al. (2016), due to a higher estimate of emissions from inland waters, highlighting the need for more detailed research on emissions factors. Priorities for improving the methane budget include (i) a global, high-resolution map of water-saturated soils and inundated areas emitting methane based on a robust classification of different types of emitting habitats; (ii) further development of process-based models for inland-water emissions; (iii) intensification of methane observations at local scales (e.g., FLUXNET-CH4 measurements) and urban-scale monitoring to constrain bottom-up land surface models, and at regional scales (surface networks and satellites) to constrain atmospheric inversions; (iv) improvements of transport models and the representation of photochemical sinks in top-down inversions; and (v) development of a 3D variational inversion system using isotopic and/or co-emitted species such as ethane to improve source partitioning. The data presented here can be downloaded from https://doi.org/10.18160/GCP-CH4-2019 (Saunois et al., 2020) and from the Global Carbon Project.

Global fire-vegetation models are widely used to assess impacts of environmental change on fire regimes and the carbon cycle and to infer relationships between climate, land use and fire. However, differences in model structure and parameterizations, in both the vegetation and fire components of these models, could influence overall model performance, and to date there has been limited evaluation of how well different models represent various aspects of fire regimes. The Fire Model Intercomparison Project (FireMIP) is coordinating the evaluation of state-of-the-art global fire models, in order to improve projections of fire characteristics and fire impacts on ecosystems and human societies in the context of global environmental change. Here we perform a systematic evaluation of historical simulations made by nine FireMIP models to quantify their ability to reproduce a range of fire and vegetation benchmarks. The FireMIP models simulate a wide range in global annual total burnt area (39–536 Mha) and global annual fire carbon emission (0.91–4.75 Pg C yr−1) for modern conditions (2002–2012), but most of the range in burnt area is within observational uncertainty (345–468 Mha). Benchmarking scores indicate that seven out of nine FireMIP models are able to represent the spatial pattern in burnt area. The models also reproduce the seasonality in burnt area reasonably well but struggle to simulate fire season length and are largely unable to represent interannual variations in burnt area. However, models that represent cropland fires see improved simulation of fire seasonality in the Northern Hemisphere. The three FireMIP models which explicitly simulate individual fires are able to reproduce the spatial pattern in number of fires, but fire sizes are too small in key regions, and this results in an underestimation of burnt area. The correct representation of spatial and seasonal patterns in vegetation appears to correlate with a better representation of burnt area. The two older fire models included in the FireMIP ensemble (LPJ–GUESS–GlobFIRM, MC2) clearly perform less well globally than other models, but it is difficult to distinguish between the remaining ensemble members; some of these models are better at representing certain aspects of the fire regime; none clearly outperforms all other models across the full range of variables assessed.

Shortwave cloud radiative effects (SWCREs), defined as the difference of the shortwave radiative flux between all-sky and clear-sky conditions at the surface, have been reported to play an important role in influencing the Earth's energy budget and temperature extremes. In this study, we employed a set of global climate models to examine the SWCRE responses to CO2, black carbon (BC) aerosols, and sulfate aerosols in boreal summer over the Northern Hemisphere. We found that CO2 causes positive SWCRE changes over most of the NH, and BC causes similar positive responses over North America, Europe, and eastern China but negative SWCRE over India and tropical Africa. When normalized by effective radiative forcing, the SWCRE from BC is roughly 3–5 times larger than that from CO2. SWCRE change is mainly due to cloud cover changes resulting from changes in relative humidity (RH) and, to a lesser extent, changes in cloud liquid water, circulation, dynamics, and stability. The SWCRE response to sulfate aerosols, however, is negligible compared to that for CO2 and BC because part of the radiation scattered by clouds under all-sky conditions will also be scattered by aerosols under clear-sky conditions. Using a multilinear regression model, it is found that mean daily maximum temperature (Tmax) increases by 0.15 and 0.13 K per watt per square meter (W m−2) increase in local SWCRE under the CO2 and BC experiment, respectively. When domain-averaged, the contribution of SWCRE change to summer mean Tmax changes was 10 %–30 % under CO2 forcing and 30 %–50 % under BC forcing, varying by region, which can have important implications for extreme climatic events and socioeconomic activities.

Projections of future atmospheric composition change and its impacts on air quality and climate depend heavily on chemistry–climate models that allow us to investigate the effects of changing emissions and meteorology. These models are imperfect as they rely on our understanding of the chemical, physical and dynamical processes governing atmospheric composition, on the approximations needed to represent these numerically, and on the limitations of the observations required to constrain them. Model intercomparison studies show substantial diversity in results that reflect underlying uncertainties, but little progress has been made in explaining the causes of this or in identifying the weaknesses in process understanding or representation that could lead to improved models and to better scientific understanding. Global sensitivity analysis provides a valuable method of identifying and quantifying the main causes of diversity in current models. For the first time, we apply Gaussian process emulation with three independent global chemistry-transport models to quantify the sensitivity of ozone and hydroxyl radicals (OH) to important climate-relevant variables, poorly characterised processes and uncertain emissions. We show a clear sensitivity of tropospheric ozone to atmospheric humidity and precursor emissions which is similar for the models, but find large differences between models for methane lifetime, highlighting substantial differences in the sensitivity of OH to primary and secondary production. This approach allows us to identify key areas where model improvements are required while providing valuable new insight into the processes driving tropospheric composition change.

Water vapour in the atmosphere is the source of a major climate feedback mechanism and potential increases in the availability of water vapour could have important consequences for mean and extreme precipitation. Future precipitation changes further depend on how the hydrological cycle responds to different drivers of climate change, such as greenhouse gases and aerosols. Currently, neither the total anthropogenic influence on the hydrological cycle nor that from individual drivers is constrained sufficiently to make solid projections. We investigate how integrated water vapour (IWV) responds to different drivers of climate change. Results from 11 global climate models have been used, based on simulations where CO2, methane, solar irradiance, black carbon (BC), and sulfate have been perturbed separately. While the global-mean IWV is usually assumed to increase by ∼7 % per kelvin of surface temperature change, we find that the feedback response of IWV differs somewhat between drivers. Fast responses, which include the initial radiative effect and rapid adjustments to an external forcing, amplify these differences. The resulting net changes in IWV range from 6.4±0.9 % K−1 for sulfate to 9.8±2 % K−1 for BC. We further calculate the relationship between global changes in IWV and precipitation, which can be characterized by quantifying changes in atmospheric water vapour lifetime. Global climate models simulate a substantial increase in the lifetime, from 8.2±0.5 to 9.9±0.7 d between 1986–2005 and 2081–2100 under a high-emission scenario, and we discuss to what extent the water vapour lifetime provides additional information compared to analysis of IWV and precipitation separately. We conclude that water vapour lifetime changes are an important indicator of changes in precipitation patterns and that BC is particularly efficient in prolonging the mean time, and therefore likely the distance, between evaporation and precipitation.

Global sensitivity analysis (GSA) is a powerful approach in identifying which inputs or parameters most affect a model's output. This determines which inputs to include when performing model calibration or uncertainty analysis. GSA allows quantification of the sensitivity index (SI) of a particular input – the percentage of the total variability in the output attributed to the changes in that input – by averaging over the other inputs rather than fixing them at specific values. Traditional methods of computing the SIs using the Sobol and extended Fourier Amplitude Sensitivity Test (eFAST) methods involve running a model thousands of times, but this may not be feasible for computationally expensive Earth system models. GSA methods that use a statistical emulator in place of the expensive model are popular, as they require far fewer model runs. We performed an eight-input GSA, using the Sobol and eFAST methods, on two computationally expensive atmospheric chemical transport models using emulators that were trained with 80 runs of the models. We considered two methods to further reduce the computational cost of GSA: (1) a dimension reduction approach and (2) an emulator-free approach. When the output of a model is multi-dimensional, it is common practice to build a separate emulator for each dimension of the output space. Here, we used principal component analysis (PCA) to reduce the output dimension, built an emulator for each of the transformed outputs, and then computed SIs of the reconstructed output using the Sobol method. We considered the global distribution of the annual column mean lifetime of atmospheric methane, which requires ∼  2000 emulators without PCA but only 5–40 emulators with PCA. We also applied an emulator-free method using a generalised additive model (GAM) to estimate the SIs using only the training runs. Compared to the emulator-only methods, the emulator–PCA and GAM methods accurately estimated the SIs of the ∼  2000 methane lifetime outputs but were on average 24 and 37 times faster, respectively.

Atmospheric aerosols and greenhouse gases affect cloud properties, radiative balance and, thus, the hydrological cycle. Observations show that precipitation has decreased in the Mediterranean since the beginning of the 20th century, and many studies have investigated possible mechanisms. So far, however, the effects of aerosol forcing on Mediterranean precipitation remain largely unknown. Here we compare the modeled dynamical response of Mediterranean precipitation to individual forcing agents in a set of global climate models (GCMs). Our analyses show that both greenhouse gases and aerosols can cause drying in the Mediterranean and that precipitation is more sensitive to black carbon (BC) forcing than to well-mixed greenhouse gases (WMGHGs) or sulfate aerosol. In addition to local heating, BC appears to reduce precipitation by causing an enhanced positive sea level pressure (SLP) pattern similar to the North Atlantic Oscillation–Arctic Oscillation, characterized by higher SLP at midlatitudes and lower SLP at high latitudes. WMGHGs cause a similar SLP change, and both are associated with a northward diversion of the jet stream and storm tracks, reducing precipitation in the Mediterranean while increasing precipitation in northern Europe. Though the applied forcings were much larger, if forcings are scaled to those of the historical period of 1901–2010, roughly one-third (31±17 %) of the precipitation decrease would be attributable to global BC forcing with the remainder largely attributable to WMGHGs, whereas global scattering sulfate aerosols would have negligible impacts. Aerosol–cloud interactions appear to have minimal impacts on Mediterranean precipitation in these models, at least in part because many simulations did not fully include such processes; these merit further study. The findings from this study suggest that future BC and WMGHG emissions may significantly affect regional water resources, agricultural practices, ecosystems and the economy in the Mediterranean region.

Following the recent Global Carbon Project (GCP) synthesis of the decadal methane (CH4) budget over 2000–2012 (Saunois et al., 2016), we analyse here the same dataset with a focus on quasi-decadal and inter-annual variability in CH4 emissions. The GCP dataset integrates results from top-down studies (exploiting atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up models (including process-based models for estimating land surface emissions and atmospheric chemistry), inventories of anthropogenic emissions, and data-driven approaches. The annual global methane emissions from top-down studies, which by construction match the observed methane growth rate within their uncertainties, all show an increase in total methane emissions over the period 2000–2012, but this increase is not linear over the 13 years. Despite differences between individual studies, the mean emission anomaly of the top-down ensemble shows no significant trend in total methane emissions over the period 2000–2006, during the plateau of atmospheric methane mole fractions, and also over the period 2008–2012, during the renewed atmospheric methane increase. However, the top-down ensemble mean produces an emission shift between 2006 and 2008, leading to 22 [16–32] Tg CH4 yr−1 higher methane emissions over the period 2008–2012 compared to 2002–2006. This emission increase mostly originated from the tropics, with a smaller contribution from mid-latitudes and no significant change from boreal regions. The regional contributions remain uncertain in top-down studies. Tropical South America and South and East Asia seem to contribute the most to the emission increase in the tropics. However, these two regions have only limited atmospheric measurements and remain therefore poorly constrained. The sectorial partitioning of this emission increase between the periods 2002–2006 and 2008–2012 differs from one atmospheric inversion study to another. However, all top-down studies suggest smaller changes in fossil fuel emissions (from oil, gas, and coal industries) compared to the mean of the bottom-up inventories included in this study. This difference is partly driven by a smaller emission change in China from the top-down studies compared to the estimate in the Emission Database for Global Atmospheric Research (EDGARv4.2) inventory, which should be revised to smaller values in a near future. We apply isotopic signatures to the emission changes estimated for individual studies based on five emission sectors and find that for six individual top-down studies (out of eight) the average isotopic signature of the emission changes is not consistent with the observed change in atmospheric 13CH4. However, the partitioning in emission change derived from the ensemble mean is consistent with this isotopic constraint. At the global scale, the top-down ensemble mean suggests that the dominant contribution to the resumed atmospheric CH4 growth after 2006 comes from microbial sources (more from agriculture and waste sectors than from natural wetlands), with an uncertain but smaller contribution from fossil CH4 emissions. In addition, a decrease in biomass burning emissions (in agreement with the biomass burning emission databases) makes the balance of sources consistent with atmospheric 13CH4 observations. In most of the top-down studies included here, OH concentrations are considered constant over the years (seasonal variations but without any inter-annual variability). As a result, the methane loss (in particular through OH oxidation) varies mainly through the change in methane concentrations and not its oxidants. For these reasons, changes in the methane loss could not be properly investigated in this study, although it may play a significant role in the recent atmospheric methane changes as briefly discussed at the end of the paper.

The important role of fire in regulating vegetation community composition and contributions to emissions of greenhouse gases and aerosols make it a critical component of dynamic global vegetation models and Earth system models. Over 2 decades of development, a wide variety of model structures and mechanisms have been designed and incorporated into global fire models, which have been linked to different vegetation models. However, there has not yet been a systematic examination of how these different strategies contribute to model performance. Here we describe the structure of the first phase of the Fire Model Intercomparison Project (FireMIP), which for the first time seeks to systematically compare a number of models. By combining a standardized set of input data and model experiments with a rigorous comparison of model outputs to each other and to observations, we will improve the understanding of what drives vegetation fire, how it can best be simulated, and what new or improved observational data could allow better constraints on model behavior. In this paper, we introduce the fire models used in the first phase of FireMIP, the simulation protocols applied, and the benchmarking system used to evaluate the models. We have also created supplementary tables that describe, in thorough mathematical detail, the structure of each model.

This paper presents a comprehensive description and benchmark evaluation of the tropospheric gas-phase chemistry component of the Multiscale Online Nonhydrostatic AtmospheRe CHemistry model (NMMB-MONARCH), formerly known as NMMB/BSC-CTM, that can be run on both regional and global domains. Here, we provide an extensive evaluation of a global annual cycle simulation using a variety of background surface stations (EMEP, WDCGG and CASTNET), ozonesondes (WOUDC, CMD and SHADOZ), aircraft data (MOZAIC and several campaigns), and satellite observations (SCIAMACHY and MOPITT). We also include an extensive discussion of our results in comparison to other state-of-the-art models. We note that in this study, we omitted aerosol processes and some natural emissions (lightning and volcano emissions). The model shows a realistic oxidative capacity across the globe. The seasonal cycle for CO is fairly well represented at different locations (correlations around 0.3–0.7 in surface concentrations), although concentrations are underestimated in spring and winter in the Northern Hemisphere, and are overestimated throughout the year at 800 and 500 hPa in the Southern Hemisphere. Nitrogen species are well represented in almost all locations, particularly NO2 in Europe (root mean square error – RMSE – below 5 ppb). The modeled vertical distributions of NOx and HNO3 are in excellent agreement with the observed values and the spatial and seasonal trends of tropospheric NO2 columns correspond well to observations from SCIAMACHY, capturing the highly polluted areas and the biomass burning cycle throughout the year. Over Asia, the model underestimates NOx from March to August, probably due to an underestimation of NOx emissions in the region. Overall, the comparison of the modeled CO and NO2 with MOPITT and SCIAMACHY observations emphasizes the need for more accurate emission rates from anthropogenic and biomass burning sources (i.e., specification of temporal variability). The resulting ozone (O3) burden (348 Tg) lies within the range of other state-of-the-art global atmospheric chemistry models. The model generally captures the spatial and seasonal trends of background surface O3 and its vertical distribution. However, the model tends to overestimate O3 throughout the troposphere in several stations. This may be attributed to an overestimation of CO concentration over the Southern Hemisphere leading to an excessive production of O3 or to the lack of specific chemistry (e.g., halogen chemistry, aerosol chemistry). Overall, O3 correlations range between 0.6 and 0.8 for daily mean values. The overall performance of the NMMB-MONARCH is comparable to that of other state-of-the-art global chemistry models.

The global methane (CH4) budget is becoming an increasingly important component for managing realistic pathways to mitigate climate change. This relevance, due to a shorter atmospheric lifetime and a stronger warming potential than carbon dioxide, is challenged by the still unexplained changes of atmospheric CH4 over the past decade. Emissions and concentrations of CH4 are continuing to increase, making CH4 the second most important human-induced greenhouse gas after carbon dioxide. Two major difficulties in reducing uncertainties come from the large variety of diffusive CH4 sources that overlap geographically, and from the destruction of CH4 by the very short-lived hydroxyl radical (OH). To address these difficulties, we have established a consortium of multi-disciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate research on the methane cycle, and producing regular (∼ biennial) updates of the global methane budget. This consortium includes atmospheric physicists and chemists, biogeochemists of surface and marine emissions, and socio-economists who study anthropogenic emissions. Following Kirschke et al. (2013), we propose here the first version of a living review paper that integrates results of top-down studies (exploiting atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up models, inventories and data-driven approaches (including process-based models for estimating land surface emissions and atmospheric chemistry, and inventories for anthropogenic emissions, data-driven extrapolations). For the 2003–2012 decade, global methane emissions are estimated by top-down inversions at 558 Tg CH4 yr−1, range 540–568. About 60 % of global emissions are anthropogenic (range 50–65 %). Since 2010, the bottom-up global emission inventories have been closer to methane emissions in the most carbon-intensive Representative Concentrations Pathway (RCP8.5) and higher than all other RCP scenarios. Bottom-up approaches suggest larger global emissions (736 Tg CH4 yr−1, range 596–884) mostly because of larger natural emissions from individual sources such as inland waters, natural wetlands and geological sources. Considering the atmospheric constraints on the top-down budget, it is likely that some of the individual emissions reported by the bottom-up approaches are overestimated, leading to too large global emissions. Latitudinal data from top-down emissions indicate a predominance of tropical emissions (∼ 64 % of the global budget, 4 yr−1, range 51–72, −14 %) and higher emissions in Africa (86 Tg CH4 yr−1, range 73–108, +19 %) than bottom-up values used as prior estimates. Overall, uncertainties for anthropogenic emissions appear smaller than those from natural sources, and the uncertainties on source categories appear larger for top-down inversions than for bottom-up inventories and models. The most important source of uncertainty on the methane budget is attributable to emissions from wetland and other inland waters. We show that the wetland extent could contribute 30–40 % on the estimated range for wetland emissions. Other priorities for improving the methane budget include the following: (i) the development of process-based models for inland-water emissions, (ii) the intensification of methane observations at local scale (flux measurements) to constrain bottom-up land surface models, and at regional scale (surface networks and satellites) to constrain top-down inversions, (iii) improvements in the estimation of atmospheric loss by OH, and (iv) improvements of the transport models integrated in top-down inversions. The data presented here can be downloaded from the Carbon Dioxide Information Analysis Center (http://doi.org/10.3334/CDIAC/GLOBAL_METHANE_BUDGET_2016_V1.1) and the Global Carbon Project.

We use the HadGEM3-GA4, CESM1, and GISS ModelE2 climate models to investigate the global and regional aerosol burden, radiative flux, and surface temperature responses to removing anthropogenic sulfur dioxide (SO2) emissions from China. We find that the models differ by up to a factor of 6 in the simulated change in aerosol optical depth (AOD) and shortwave radiative flux over China that results from reduced sulfate aerosol, leading to a large range of magnitudes in the regional and global temperature responses. Two of the three models simulate a near-ubiquitous hemispheric warming due to the regional SO2 removal, with similarities in the local and remote pattern of response, but overall with a substantially different magnitude. The third model simulates almost no significant temperature response. We attribute the discrepancies in the response to a combination of substantial differences in the chemical conversion of SO2 to sulfate, translation of sulfate mass into AOD, cloud radiative interactions, and differences in the radiative forcing efficiency of sulfate aerosol in the models. The model with the strongest response (HadGEM3-GA4) compares best with observations of AOD regionally, however the other two models compare similarly (albeit poorly) and still disagree substantially in their simulated climate response, indicating that total AOD observations are far from sufficient to determine which model response is more plausible. Our results highlight that there remains a large uncertainty in the representation of both aerosol chemistry as well as direct and indirect aerosol radiative effects in current climate models, and reinforces that caution must be applied when interpreting the results of modelling studies of aerosol influences on climate. Model studies that implicate aerosols in climate responses should ideally explore a range of radiative forcing strengths representative of this uncertainty, in addition to thoroughly evaluating the models used against observations.

Warm and dry climatological conditions favour the occurrence of forest fires. These fires then become a significant emission source to the atmosphere. Despite this global importance, fires are a local phenomenon and are difficult to represent in large-scale Earth system models (ESMs). To address this, the INteractive Fire and Emission algoRithm for Natural envirOnments (INFERNO) was developed. INFERNO follows a reduced complexity approach and is intended for decadal- to centennial-scale climate simulations and assessment models for policy making. Fuel flammability is simulated using temperature, relative humidity (RH) and fuel load as well as precipitation and soil moisture. Combining flammability with ignitions and vegetation, the burnt area is diagnosed. Emissions of carbon and key species are estimated using the carbon scheme in the Joint UK Land Environment Simulator (JULES) land surface model. JULES also possesses fire index diagnostics, which we document and compare with our fire scheme. We found INFERNO captured global burnt area variability better than individual indices, and these performed best for their native regions. Two meteorology data sets and three ignition modes are used to validate the model. INFERNO is shown to effectively diagnose global fire occurrence (R = 0.66) and emissions (R = 0.59) through an approach appropriate to the complexity of an ESM, although regional biases remain.

Biomass burning impacts vegetation dynamics, biogeochemical cycling, atmospheric chemistry, and climate, with sometimes deleterious socio-economic impacts. Under future climate projections it is often expected that the risk of wildfires will increase. Our ability to predict the magnitude and geographic pattern of future fire impacts rests on our ability to model fire regimes, using either well-founded empirical relationships or process-based models with good predictive skill. While a large variety of models exist today, it is still unclear which type of model or degree of complexity is required to model fire adequately at regional to global scales. This is the central question underpinning the creation of the Fire Model Intercomparison Project (FireMIP), an international initiative to compare and evaluate existing global fire models against benchmark data sets for present-day and historical conditions. In this paper we review how fires have been represented in fire-enabled dynamic global vegetation models (DGVMs) and give an overview of the current state of the art in fire-regime modelling. We indicate which challenges still remain in global fire modelling and stress the need for a comprehensive model evaluation and outline what lessons may be learned from FireMIP.

In this paper, we present a description of the tropospheric chemistry component of the UK Chemistry and Aerosols (UKCA) model which has been coupled to the Met Office Hadley Centre's HadGEM family of climate models. We assess the model's transport and scavenging processes, in particular focussing on convective transport, boundary layer mixing, wet scavenging and inter-hemispheric exchange. Simulations with UKCA of the short-lived radon tracer suggest that modelled distributions are comparable to those of other models and the comparison with observations indicate that apart from a few locations, boundary layer mixing and convective transport are effective in the model as a means of vertically redistributing surface emissions of radon. Comparisons of modelled lead tracer concentrations with observations suggest that UKCA captures surface concentrations in both hemispheres very well, although there is a tendency to underestimate the observed geographical and interannual variability in the Northern Hemisphere. In particular, UKCA replicates the shape and absolute concentrations of observed lead profiles, a key test in the evaluation of a model's wet scavenging scheme. The timescale for inter-hemispheric transport, calculated in the model using a simple krypton tracer experiment, does appear to be long relative to other models and could indicate deficiencies in tropical deep convection and/or insufficient boundary layer mixing. We also describe the main components of the tropospheric chemistry and evaluate it against observations and other tropospheric chemistry models. In particular, from a climate forcing perspective, present-day observed surface methane concentrations and tropospheric ozone concentrations are reproduced very well by the model, thereby making it suitable for long centennial integrations as well as studies of biogeochemical feedbacks. Results from both historical and future simulations with UKCA tropospheric chemistry are presented. Future projections of tropospheric ozone vary with the Representative Concentration Pathway (RCP). In RCP2.6, for example, tropospheric ozone increases up to 2010 and then declines by 13% of its year-2000 global mean by the end of the century. In RCP8.5, tropospheric ozone continues to rise steadily throughout the 21st century, with methane being the main driving factor. Finally, we highlight aspects of the UKCA model which are undergoing and/or have undergone recent developments and are suitable for inclusion in a next-generation Earth System Model.

We have analysed time-slice simulations from 17 global models, participating in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP), to explore changes in present-day (2000) hydroxyl radical (OH) concentration and methane (CH4) lifetime relative to preindustrial times (1850) and to 1980. A comparison of modeled and observation-derived methane and methyl chloroform lifetimes suggests that the present-day global multi-model mean OH concentration is overestimated by 5 to 10% but is within the range of uncertainties. The models consistently simulate higher OH concentrations in the Northern Hemisphere (NH) compared with the Southern Hemisphere (SH) for the present-day (2000; inter-hemispheric ratios of 1.13 to 1.42), in contrast to observation-based approaches which generally indicate higher OH in the SH although uncertainties are large. Evaluation of simulated carbon monoxide (CO) concentrations, the primary sink for OH, against ground-based and satellite observations suggests low biases in the NH that may contribute to the high north–south OH asymmetry in the models. The models vary widely in their regional distribution of present-day OH concentrations (up to 34%). Despite large regional changes, the multi-model global mean (mass-weighted) OH concentration changes little over the past 150 yr, due to concurrent increases in factors that enhance OH (humidity, tropospheric ozone, nitrogen oxide (NOx) emissions, and UV radiation due to decreases in stratospheric ozone), compensated by increases in OH sinks (methane abundance, carbon monoxide and non-methane volatile organic carbon (NMVOC) emissions). The large inter-model diversity in the sign and magnitude of preindustrial to present-day OH changes (ranging from a decrease of 12.7% to an increase of 14.6%) indicate that uncertainty remains in our understanding of the long-term trends in OH and methane lifetime. We show that this diversity is largely explained by the different ratio of the change in global mean tropospheric CO and NOx burdens (ΔCO/ΔNOx, approximately represents changes in OH sinks versus changes in OH sources) in the models, pointing to a need for better constraints on natural precursor emissions and on the chemical mechanisms in the current generation of chemistry-climate models. For the 1980 to 2000 period, we find that climate warming and a slight increase in mean OH (3.5 ± 2.2%) leads to a 4.3 ± 1.9% decrease in the methane lifetime. Analysing sensitivity simulations performed by 10 models, we find that preindustrial to present-day climate change decreased the methane lifetime by about four months, representing a negative feedback on the climate system. Further, we analysed attribution experiments performed by a subset of models relative to 2000 conditions with only one precursor at a time set to 1860 levels. We find that global mean OH increased by 46.4 ± 12.2% in response to preindustrial to present-day anthropogenic NOx emission increases, and decreased by 17.3 ± 2.3%, 7.6 ± 1.5%, and 3.1 ± 3.0% due to methane burden, and anthropogenic CO, and NMVOC emissions increases, respectively.

Coupling between the stratosphere and the troposphere allows changes in stratospheric ozone abundances to affect tropospheric chemistry. Large-scale effects from such changes on chemically produced tropospheric aerosols have not been systematically examined in past studies. We use a composition-climate model to investigate potential past and future impacts of changes in stratospheric ozone depleting substances (ODS) on tropospheric oxidants and sulfate aerosols. In most experiments, we find significant responses in tropospheric photolysis and oxidants, with small but significant effects on methane radiative forcing. The response of sulfate aerosols is sizeable when examining the effect of increasing future nitrous oxide (N2O) emissions. We also find that without the regulation of chlorofluorocarbons (CFCs) through the Montreal Protocol, sulfate aerosols could have increased by 2050 by a comparable amount to the decreases predicted due to relatively stringent sulfur emissions controls. The individual historical radiative forcings of CFCs and N2O through their indirect effects on methane (−22.6 mW m−2 for CFCs and −6.7 mW m−2 for N2O) and sulfate aerosols (−3.0 mW m−2 for CFCs and +6.5 mW m−2 for N2O when considering the direct aerosol effect) discussed here are non-negligible when compared to known historical ODS forcing. Our results stress the importance of accounting for stratosphere-troposphere, gas-aerosol and composition-climate interactions when investigating the effects of changing emissions on atmospheric composition and climate.

We use simultaneous observations of tropospheric ozone and outgoing longwave radiation (OLR) sensitivity to tropospheric ozone from the Tropospheric Emission Spectrometer (TES) to evaluate model tropospheric ozone and its effect on OLR simulated by a suite of chemistry-climate models that participated in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). The ensemble mean of ACCMIP models show a persistent but modest tropospheric ozone low bias (5–20 ppb) in the Southern Hemisphere (SH) and modest high bias (5–10 ppb) in the Northern Hemisphere (NH) relative to TES ozone for 2005–2010. These ozone biases have a significant impact on the OLR. Using TES instantaneous radiative kernels (IRK), we show that the ACCMIP ensemble mean tropospheric ozone low bias leads up to 120 mW m−2 OLR high bias locally but zonally compensating errors reduce the global OLR high bias to 39 ± 41 m Wm−2 relative to TES data. We show that there is a correlation (R2 = 0.59) between the magnitude of the ACCMIP OLR bias and the deviation of the ACCMIP preindustrial to present day (1750–2010) ozone radiative forcing (RF) from the ensemble ozone RF mean. However, this correlation is driven primarily by models whose absolute OLR bias from tropospheric ozone exceeds 100 m Wm−2. Removing these models leads to a mean ozone radiative forcing of 394 ± 42 m Wm−2. The mean is about the same and the standard deviation is about 30% lower than an ensemble ozone RF of 384 ± 60 m Wm−2 derived from 14 of the 16 ACCMIP models reported in a companion ACCMIP study. These results point towards a profitable direction of combining satellite observations and chemistry-climate model simulations to reduce uncertainty in ozone radiative forcing.

The Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) examined the short-lived drivers of climate change in current climate models. Here we evaluate the 10 ACCMIP models that included aerosols, 8 of which also participated in the Coupled Model Intercomparison Project phase 5 (CMIP5). The models reproduce present-day total aerosol optical depth (AOD) relatively well, though many are biased low. Contributions from individual aerosol components are quite different, however, and most models underestimate east Asian AOD. The models capture most 1980–2000 AOD trends well, but underpredict increases over the Yellow/Eastern Sea. They strongly underestimate absorbing AOD in many regions. We examine both the direct radiative forcing (RF) and the forcing including rapid adjustments (effective radiative forcing; ERF, including direct and indirect effects). The models' all-sky 1850 to 2000 global mean annual average total aerosol RF is (mean; range) −0.26 W m−2; −0.06 to −0.49 W m−2. Screening based on model skill in capturing observed AOD yields a best estimate of −0.42 W m−2; −0.33 to −0.50 W m−2, including adjustment for missing aerosol components in some models. Many ACCMIP and CMIP5 models appear to produce substantially smaller aerosol RF than this best estimate. Climate feedbacks contribute substantially (35 to −58%) to modeled historical aerosol RF. The 1850 to 2000 aerosol ERF is −1.17 W m−2; −0.71 to −1.44 W m−2. Thus adjustments, including clouds, typically cause greater forcing than direct RF. Despite this, the multi-model spread relative to the mean is typically the same for ERF as it is for RF, or even smaller, over areas with substantial forcing. The largest 1850 to 2000 negative aerosol RF and ERF values are over and near Europe, south and east Asia and North America. ERF, however, is positive over the Sahara, the Karakoram, high Southern latitudes and especially the Arctic. Global aerosol RF peaks in most models around 1980, declining thereafter with only weak sensitivity to the Representative Concentration Pathway (RCP). One model, however, projects approximately stable RF levels, while two show increasingly negative RF due to nitrate (not included in most models). Aerosol ERF, in contrast, becomes more negative during 1980 to 2000. During this period, increased Asian emissions appear to have a larger impact on aerosol ERF than European and North American decreases due to their being upwind of the large, relatively pristine Pacific Ocean. There is no clear relationship between historical aerosol ERF and climate sensitivity in the CMIP5 subset of ACCMIP models. In the ACCMIP/CMIP5 models, historical aerosol ERF of about −0.8 to −1.5 W m−2 is most consistent with observed historical warming. Aerosol ERF masks a large portion of greenhouse forcing during the late 20th and early 21st century at the global scale. Regionally, aerosol ERF is so large that net forcing is negative over most industrialized and biomass burning regions through 1980, but remains strongly negative only over east and southeast Asia by 2000. Net forcing is strongly positive by 1980 over most deserts, the Arctic, Australia, and most tropical oceans. Both the magnitude of and area covered by positive forcing expand steadily thereafter.

Ozone (O3) from 17 atmospheric chemistry models taking part in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) has been used to calculate tropospheric ozone radiative forcings (RFs). All models applied a common set of anthropogenic emissions, which are better constrained for the present-day than the past. Future anthropogenic emissions follow the four Representative Concentration Pathway (RCP) scenarios, which define a relatively narrow range of possible air pollution emissions. We calculate a value for the pre-industrial (1750) to present-day (2010) tropospheric ozone RF of 410 mW m−2. The model range of pre-industrial to present-day changes in O3 produces a spread (±1 standard deviation) in RFs of ±17%. Three different radiation schemes were used – we find differences in RFs between schemes (for the same ozone fields) of ±10%. Applying two different tropopause definitions gives differences in RFs of ±3%. Given additional (unquantified) uncertainties associated with emissions, climate-chemistry interactions and land-use change, we estimate an overall uncertainty of ±30% for the tropospheric ozone RF. Experiments carried out by a subset of six models attribute tropospheric ozone RF to increased emissions of methane (44±12%), nitrogen oxides (31 ± 9%), carbon monoxide (15 ± 3%) and non-methane volatile organic compounds (9 ± 2%); earlier studies attributed more of the tropospheric ozone RF to methane and less to nitrogen oxides. Normalising RFs to changes in tropospheric column ozone, we find a global mean normalised RF of 42 mW m−2 DU−1, a value similar to previous work. Using normalised RFs and future tropospheric column ozone projections we calculate future tropospheric ozone RFs (mW m−2; relative to 1750) for the four future scenarios (RCP2.6, RCP4.5, RCP6.0 and RCP8.5) of 350, 420, 370 and 460 (in 2030), and 200, 300, 280 and 600 (in 2100). Models show some coherent responses of ozone to climate change: decreases in the tropical lower troposphere, associated with increases in water vapour; and increases in the sub-tropical to mid-latitude upper troposphere, associated with increases in lightning and stratosphere-to-troposphere transport. Climate change has relatively small impacts on global mean tropospheric ozone RF.

The new generation GISS climate model includes fully interactive chemistry related to ozone in historical and future simulations, and interactive methane in future simulations. Evaluation of ozone, its tropospheric precursors, and methane shows that the model captures much of the large-scale spatial structure seen in recent observations. While the model is much improved compared with the previous chemistry-climate model, especially for ozone seasonality in the stratosphere, there is still slightly too rapid stratospheric circulation, too little stratosphere-to-troposphere ozone flux in the Southern Hemisphere and an Antarctic ozone hole that is too large and persists too long. Quantitative metrics of spatial and temporal correlations with satellite datasets as well as spatial autocorrelation to examine transport and mixing are presented to document improvements in model skill and provide a benchmark for future evaluations. The difference in radiative forcing (RF) calculated using modeled tropospheric ozone versus tropospheric ozone observed by TES is only 0.016 W m−2. Historical 20th Century simulations show a steady increase in whole atmosphere ozone RF through 1970 after which there is a decrease through 2000 due to stratospheric ozone depletion. Ozone forcing increases throughout the 21st century under RCP8.5 owing to a projected recovery of stratospheric ozone depletion and increases in methane, but decreases under RCP4.5 and 2.6 due to reductions in emissions of other ozone precursors. RF from methane is 0.05 to 0.18 W m−2 higher in our model calculations than in the RCP RF estimates. The surface temperature response to ozone through 1970 follows the increase in forcing due to tropospheric ozone. After that time, surface temperatures decrease as ozone RF declines due to stratospheric depletion. The stratospheric ozone depletion also induces substantial changes in surface winds and the Southern Ocean circulation, which may play a role in a slightly stronger response per unit forcing during later decades. Tropical precipitation shifts south during boreal summer from 1850 to 1970, but then shifts northward from 1970 to 2000, following upper tropospheric temperature gradients more strongly than those at the surface.

Results from simulations performed for the Atmospheric Chemistry and Climate Modeling Intercomparison Project (ACCMIP) are analysed to examine how OH and methane lifetime may change from present day to the future, under different climate and emissions scenarios. Present day (2000) mean tropospheric chemical lifetime derived from the ACCMIP multi-model mean is 9.8 ± 1.6 yr (9.3 ± 0.9 yr when only including selected models), lower than a recent observationally-based estimate, but with a similar range to previous multi-model estimates. Future model projections are based on the four Representative Concentration Pathways (RCPs), and the results also exhibit a large range. Decreases in global methane lifetime of 4.5 ± 9.1% are simulated for the scenario with lowest radiative forcing by 2100 (RCP 2.6), while increases of 8.5 ± 10.4% are simulated for the scenario with highest radiative forcing (RCP 8.5). In this scenario, the key driver of the evolution of OH and methane lifetime is methane itself, since its concentration more than doubles by 2100 and it consumes much of the OH that exists in the troposphere. Stratospheric ozone recovery, which drives tropospheric OH decreases through photolysis modifications, also plays a partial role. In the other scenarios, where methane changes are less drastic, the interplay between various competing drivers leads to smaller and more diverse OH and methane lifetime responses, which are difficult to attribute. For all scenarios, regional OH changes are even more variable, with the most robust feature being the large decreases over the remote oceans in RCP8.5. Through a regression analysis, we suggest that differences in emissions of non-methane volatile organic compounds and in the simulation of photolysis rates may be the main factors causing the differences in simulated present day OH and methane lifetime. Diversity in predicted changes between present day and future OH was found to be associated more strongly with differences in modelled temperature and stratospheric ozone changes. Finally, through perturbation experiments we calculated an OH feedback factor (F) of 1.24 from present day conditions (1.50 from 2100 RCP8.5 conditions) and a climate feedback on methane lifetime of 0.33 ± 0.13 yr K−1, on average. Models that did not include interactive stratospheric ozone effects on photolysis showed a stronger sensitivity to climate, as they did not account for negative effects of climate-driven stratospheric ozone recovery on tropospheric OH, which would have partly offset the overall OH/methane lifetime response to climate change.

The Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) consists of a series of time slice experiments targeting the long-term changes in atmospheric composition between 1850 and 2100, with the goal of documenting composition changes and the associated radiative forcing. In this overview paper, we introduce the ACCMIP activity, the various simulations performed (with a requested set of 14) and the associated model output. The 16 ACCMIP models have a wide range of horizontal and vertical resolutions, vertical extent, chemistry schemes and interaction with radiation and clouds. While anthropogenic and biomass burning emissions were specified for all time slices in the ACCMIP protocol, it is found that the natural emissions are responsible for a significant range across models, mostly in the case of ozone precursors. The analysis of selected present-day climate diagnostics (precipitation, temperature, specific humidity and zonal wind) reveals biases consistent with state-of-the-art climate models. The model-to-model comparison of changes in temperature, specific humidity and zonal wind between 1850 and 2000 and between 2000 and 2100 indicates mostly consistent results. However, models that are clear outliers are different enough from the other models to significantly affect their simulation of atmospheric chemistry.

Present day tropospheric ozone and its changes between 1850 and 2100 are considered, analysing 15 global models that participated in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). The ensemble mean compares well against present day observations. The seasonal cycle correlates well, except for some locations in the tropical upper troposphere. Most (75 %) of the models are encompassed with a range of global mean tropospheric ozone column estimates from satellite data, but there is a suggestion of a high bias in the Northern Hemisphere and a low bias in the Southern Hemisphere, which could indicate deficiencies with the ozone precursor emissions. Compared to the present day ensemble mean tropospheric ozone burden of 337 ± 23 Tg, the ensemble mean burden for 1850 time slice is ~30% lower. Future changes were modelled using emissions and climate projections from four Representative Concentration Pathways (RCPs). Compared to 2000, the relative changes in the ensemble mean tropospheric ozone burden in 2030 (2100) for the different RCPs are: −4% (−16%) for RCP2.6, 2% (−7%) for RCP4.5, 1% (−9%) for RCP6.0, and 7% (18%) for RCP8.5. Model agreement on the magnitude of the change is greatest for larger changes. Reductions in most precursor emissions are common across the RCPs and drive ozone decreases in all but RCP8.5, where doubled methane and a 40–150% greater stratospheric influx (estimated from a subset of models) increase ozone. While models with a high ozone burden for the present day also have high ozone burdens for the other time slices, no model consistently predicts large or small ozone changes; i.e. the magnitudes of the burdens and burden changes do not appear to be related simply, and the models are sensitive to emissions and climate changes in different ways. Spatial patterns of ozone changes are well correlated across most models, but are notably different for models without time evolving stratospheric ozone concentrations. A unified approach to ozone budget specifications and a rigorous investigation of the factors that drive tropospheric ozone is recommended to help future studies attribute ozone changes and inter-model differences more clearly.

Retrievals of the isotopic composition of water vapor from the Aura Tropospheric Emission Spectrometer (TES) have unique value in constraining moist processes in climate models. Accurate comparison between simulated and retrieved values requires that model profiles that would be poorly retrieved are excluded, and that an instrument operator be applied to the remaining profiles. Typically, this is done by sampling model output at satellite measurement points and using the quality flags and averaging kernels from individual retrievals at specific places and times. This approach is not reliable when the model meteorological conditions influencing retrieval sensitivity are different from those observed by the instrument at short time scales, which will be the case for free-running climate simulations. In this study, we describe an alternative, "categorical" approach to applying the instrument operator, implemented within the NASA GISS ModelE general circulation model. Retrieval quality and averaging kernel structure are predicted empirically from model conditions, rather than obtained from collocated satellite observations. This approach can be used for arbitrary model configurations, and requires no agreement between satellite-retrieved and model meteorology at short time scales. To test this approach, nudged simulations were conducted using both the retrieval-based and categorical operators. Cloud cover, surface temperature and free-tropospheric moisture content were the most important predictors of retrieval quality and averaging kernel structure. There was good agreement between the δD fields after applying the retrieval-based and more detailed categorical operators, with increases of up to 30‰ over the ocean and decreases of up to 40‰ over land relative to the raw model fields. The categorical operator performed better over the ocean than over land, and requires further refinement for use outside of the tropics. After applying the TES operator, ModelE had δD biases of −8‰ over ocean and −34‰ over land compared to TES δD, which were less than the biases using raw model δD fields.

Precipitation shifts can have large impacts on human society and ecosystems. Many aspects of how inhomogeneous radiative forcings influence precipitation remain unclear, however. Here we investigate regional precipitation responses to various forcings imposed in different latitude bands in a climate model. We find that several regions show strong, significant responses to most forcings, but that the magnitude and even the sign depends upon the forcing location and type. Aerosol and ozone forcings typically induce larger responses than equivalent carbon dioxide (CO2) forcing, and the influence of remote forcings often outweighs that of local forcings. Consistent with this, ozone and especially aerosols contribute greatly to precipitation changes over the Sahel and South and East Asia in historical simulations, and inclusion of aerosols greatly increases the agreement with observed trends in these areas, which cannot be attributed to either greenhouse gases or natural forcings. Estimates of precipitation responses derived from multiplying our Regional Precipitation Potentials (RPP; the response per unit forcing relationships) by historical forcings typically capture the actual response in full transient climate simulations fairly well, suggesting that these relationships may provide useful metrics. The strong sensitivity to aerosol and ozone forcing suggests that although some air quality improvements may unmask greenhouse gas-induced warming, they have large benefits for reducing regional disruption of the hydrologic cycle.

The correlation between measured tropospheric ozone (O3) and carbon monoxide (CO) has been used extensively in tropospheric chemistry studies to explore the photochemical characteristics of different regions and to evaluate the ability of models to capture these characteristics. Here, we present the first study that uses multi-year, global, vertically resolved, simultaneous and collocated O3 and CO satellite (Tropospheric Emission Spectrometer) measurements, to determine this correlation in the middle/lower free troposphere for two different seasons, and to evaluate two chemistry-climate models. We find results that are fairly robust across different years, altitudes and timescales considered, which indicates that the correlation maps presented here could be used in future model evaluations. The highest positive correlations (around 0.8) are found in the northern Pacific during summer, which is a common feature in the observations and the G-PUCCINI model. We make quantitative comparisons between the models using a single-figure metric (C), which we define as the correlation coefficient between the modeled and the observed O3-CO correlations for different regions of the globe. On a global scale, the G-PUCCINI model shows a good performance in the summer (C=0.71) and a satisfactory performance in the winter (C=0.52). It captures midlatitude features very well, especially in the summer, whereas the performance in regions like South America or Central Africa is weaker. The UKCA model (C=0.46/0.15 for July–August/December–January on a global scale) performs better in certain regions, such as the tropics in winter, and it captures some of the broad characteristics of summer extratropical correlations, but it systematically underestimates the O3-CO correlations over much of the globe. It is noteworthy that the correlations look very different in the two models, even though the ozone distributions are similar. This demonstrates that this technique provides a powerful global constraint for understanding modeled tropospheric chemical processes. We investigated the sources of the correlations by performing a series of sensitivity experiments. In these, the sign of the correlation is, in most cases, insensitive to removing different individual emissions, but its magnitude changes downwind of emission regions when applying such perturbations. Interestingly, we find that the O3-CO correlation does not solely reflect the strength of O3 photochemical production, as often assumed by earlier studies, but is more complicated and may reflect a mixture of different processes such as transport.

We have run a chemistry transport model (CTM) to systematically examine the drivers of interannual variability of tropospheric composition during 1996–2000. This period was characterised by anomalous meteorological conditions associated with the strong El Niño of 1997–1998 and intense wildfires, which produced a large amount of pollution. On a global scale, changing meteorology (winds, temperatures, humidity and clouds) is found to be the most important factor driving interannual variability of NO2 and ozone on the timescales considered. Changes in stratosphere-troposphere exchange, which are largely driven by meteorological variability, are found to play a particularly important role in driving ozone changes. The strong influence of emissions on NO2 and ozone interannual variability is largely confined to areas where intense biomass burning events occur. For CO, interannual variability is almost solely driven by emission changes, while for OH meteorology dominates, with the radiative influence of clouds being a very strong contributor. Through a simple attribution analysis for 1996–2000 we conclude that changing cloudiness drives 25% of the interannual variability of OH over Europe by affecting shortwave radiation. Over Indonesia this figure is as high as 71%. Changes in cloudiness contribute a small but non-negligible amount (up to 6%) to the interannual variability of ozone over Europe and Indonesia. This suggests that future assessments of trends in tropospheric oxidizing capacity should account for interannual variability in cloudiness, a factor neglected in many previous studies.

We use a three-dimensional chemical transport model to examine the shortwave radiative effects of clouds on the tropospheric ozone budget. In addition to looking at changes in global concentrations as previous studies have done, we examine changes in ozone chemical production and loss caused by clouds and how these vary in different parts of the troposphere. On a global scale, we find that clouds have a modest effect on ozone chemistry, but on a regional scale their role is much more significant, with the size of the response dependent on the region. The largest averaged changes in chemical budgets (±10–14%) are found in the marine troposphere, where cloud optical depths are high. We demonstrate that cloud effects are small on average in the middle troposphere because this is a transition region between reduction and enhancement in photolysis rates. We show that increases in boundary layer ozone due to clouds are driven by large-scale changes in downward ozone transport from higher in the troposphere rather than by decreases in in-situ ozone chemical loss rates. Increases in upper tropospheric ozone are caused by higher production rates due to backscattering of radiation and consequent increases in photolysis rates, mainly J(NO2). The global radiative effect of clouds on isoprene, through decreases of OH in the lower troposphere, is stronger than on ozone. Tropospheric isoprene lifetime increases by 7% when taking clouds into account. We compare the importance of clouds in contributing to uncertainties in the global ozone budget with the role of other radiatively-important factors. The budget is most sensitive to the overhead ozone column, while surface albedo and clouds have smaller effects. However, uncertainty in representing the spatial distribution of clouds may lead to a large sensitivity of the ozone budget components on regional scales.

A new version of the p-TOMCAT Chemical Transport Model (CTM) which includes an improved photolysis code, Fast-JX, is validated. Through offline testing we show that Fast-JX captures well the observed J(NO2) and J(O1D) values obtained at Weybourne and during a flight above the Atlantic, though with some overestimation of J(O1D) when comparing to the aircraft data. By comparing p-TOMCAT output of CO and ozone with measurements, we find that the inclusion of Fast-JX in the CTM strongly improves the latter's ability to capture the seasonality and levels of tracers' concentrations. A probability distribution analysis demonstrates that photolysis rates and oxidant (OH, ozone) concentrations cover a broader range of values when using Fast-JX instead of the standard photolysis scheme. This is not only driven by improvements in the seasonality of cloudiness but also even more by the better representation of cloud spatial variability. We use three different cloud treatments to study the radiative effect of clouds on the abundances of a range of tracers and find only modest effects on a global scale. This is consistent with the most relevant recent study. The new version of the validated CTM will be used for a variety of future studies examining the variability of tropospheric composition and its drivers.

No abstract available.