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The evolution of tropospheric ozone from 1850 to 2100 has been studied using data from Phase 6 of the Coupled Model Intercomparison Project (CMIP6). We evaluate long-term changes using coupled atmosphere–ocean chemistry–climate models, focusing on the CMIP Historical and ScenarioMIP ssp370 experiments, for which detailed tropospheric-ozone diagnostics were archived. The model ensemble has been evaluated against a suite of surface, sonde and satellite observations of the past several decades and found to reproduce well the salient spatial, seasonal and decadal variability and trends. The multi-model mean tropospheric-ozone burden increases from 247 ± 36 Tg in 1850 to a mean value of 356 ± 31 Tg for the period 2005–2014, an increase of 44 %. Modelled present-day values agree well with previous determinations (ACCENT: 336 ± 27 Tg; Atmospheric Chemistry and Climate Model Intercomparison Project, ACCMIP: 337 ± 23 Tg; Tropospheric Ozone Assessment Report, TOAR: 340 ± 34 Tg). In the ssp370 experiments, the ozone burden increases to 416 ± 35 Tg by 2100. The ozone budget has been examined over the same period using lumped ozone production (PO3) and loss (LO3) diagnostics. Both ozone production and chemical loss terms increase steadily over the period 1850 to 2100, with net chemical production (PO3-LO3) reaching a maximum around the year 2000. The residual term, which contains contributions from stratosphere–troposphere transport reaches a minimum around the same time before recovering in the 21st century, while dry deposition increases steadily over the period 1850–2100. Differences between the model residual terms are explained in terms of variation in tropopause height and stratospheric ozone burden.

Methane, a potent greenhouse gas, is a significant contributor to global warming, with future increases in its abundance potentially leading to an increase of more than 1 ∘ C by 2050 beyond other greenhouse gases if left unaddressed. To remain within the crucial target of limiting global warming to 1.5 ∘ C, it is imperative to evaluate the potential of methane removal techniques. This study presents a scoping analysis of different catalytic technologies (thermal, photochemical and electrochemical) and materials to evaluate potential limitations and energy requirements. An analysis of mass transport and reaction rates is conducted for atmospheric methane conversion system configurations. For the vast majority of catalytic technologies, the reaction rates limit the conversion which motivates future efforts for catalyst development. An analysis of energy requirements for atmospheric methane conversion shows minimum energy configurations for various catalytic technologies within classic tube or parallel plate architectures that have analogs to ventilation and industrial fins. Methane concentrations ranging from 2 ppm (ambient) to 1000 ppm (sources, such as wetlands, fossil-fuel extraction sites, landfills etc) are examined. The study finds that electrocatalysis offers the most energy efficient approach (∼0.2 GJ tonne −1 CO 2 e) for new installations in turbulent ducts, with a total energy intensity < 1 GJ tonne −1 CO 2 e. Photocatalytic methane removal catalysts are moderately more energy intensive (∼2 GJ tonne −1 CO 2 e), but could derive much of their energy input from ‘free’ solar energy sources. Thermal systems are shown to be excessively energy intensive ( > 100 GJ tonne −1 ), while combining photovoltaics with electrochemical catalysts (∼1 GJ tonne −1 CO 2 e) have comparable energy intensity to photocatalytic methane removal catalysts.

A stratosphere-resolving configuration of the Met Office's Unified Model (UM) with the United Kingdom Chemistry and Aerosols (UKCA) scheme is used to investigate the atmospheric response to changes in (a) greenhouse gases and climate, (b) ozone-depleting substances (ODSs) and (c) non-methane ozone precursor emissions. A suite of time-slice experiments show the separate, as well as pairwise, impacts of these perturbations between the years 2000 and 2100. Sensitivity to uncertainties in future greenhouse gases and aerosols is explored through the use of the Representative Concentration Pathway (RCP) 4.5 and 8.5 scenarios. The results highlight an important role for the stratosphere in determining the annual mean tropospheric ozone response, primarily through stratosphere–troposphere exchange (STE) of ozone. Under both climate change and reductions in ODSs, increases in STE offset decreases in net chemical production and act to increase the tropospheric ozone burden. This opposes the effects of projected decreases in ozone precursors through measures to improve air quality, which act to reduce the ozone burden. The global tropospheric lifetime of ozone (τO3) does not change significantly under climate change at RCP4.5, but it decreases at RCP8.5. This opposes the increases in τO3 simulated under reductions in ODSs and ozone precursor emissions. The additivity of the changes in ozone is examined by comparing the sum of the responses in the single-forcing experiments to those from equivalent combined-forcing experiments. Whilst the ozone responses to most forcing combinations are found to be approximately additive, non-additive changes are found in both the stratosphere and troposphere when a large climate forcing (RCP8.5) is combined with the effects of ODSs.

The Montreal Protocol has succeeded in limiting major ozone-depleting substance emissions, and consequently stratospheric ozone concentrations are expected to recover this century. However, there is a large uncertainty in the rate of regional ozone recovery in the Northern Hemisphere. Here we identify a Eurasia-North America dipole mode in the total column ozone over the Northern Hemisphere, showing negative and positive total column ozone anomaly centres over Eurasia and North America, respectively. The positive trend of this mode explains an enhanced total column ozone decline over the Eurasian continent in the past three decades, which is closely related to the polar vortex shift towards Eurasia. Multiple chemistry-climate-model simulations indicate that the positive Eurasia-North America dipole trend in late winter is likely to continue in the near future. Our findings suggest that the anticipated ozone recovery in late winter will be sensitive not only to the ozone-depleting substance decline but also to the polar vortex changes, and could be substantially delayed in some regions of the Northern Hemisphere extratropics. Climate change can exert a significant effect on the ozone recovery. Here, the authors show that the Arctic polar vortex shift associated with Arctic sea-ice loss could slow down ozone recovery over the Eurasian continent.

Mitigation of greenhouse gas emissions is crucial for achieving the goals of the Paris climate agreement. One key gas is methane, whose representation in most climate models is limited by using prescribed surface concentrations. Here we use a new, methane emissions-driven version of the UK Earth System Model (UKESM1) and simulate a zero anthropogenic methane emissions scenario (ZAME) in order to (i) attribute the role of anthropogenic methane emissions on the Earth system and (ii) bracket the potential for theoretical maximum mitigation. We find profound, rapid and sustained impacts on atmospheric composition and climate, compared to a counterfactual projection (SSP3-7.0, the ’worst case’ scenario for methane). In ZAME, methane declines to below pre-industrial levels within 12 years and global surface ozone decreases to levels seen in the 1970s. By 2050, 690,000 premature deaths per year and 1° of warming can be attributed to anthropogenic methane in SSP3-7.0. This work demonstrates the significant maximum potential of methane emissions reductions, and their air-quality co-benefits, but also reiterates the need for action on carbon dioxide (CO 2 ) emissions. We show that a methane emissions-driven treatment is essential for simulating the full Earth system impacts and feedbacks of methane emissions changes.

We provide an overview of the REF-C1SD specified-dynamics experiment that was conducted as part of phase 1 of the Chemistry-Climate Model Initiative (CCMI). The REF-C1SD experiment, which consisted of mainly nudged general circulation models (GCMs) constrained with (re)analysis fields, was designed to examine the influence of the large-scale circulation on past trends in atmospheric composition. The REF-C1SD simulations were produced across various model frameworks and are evaluated in terms of how well they represent different measures of the dynamical and transport circulations. In the troposphere there are large (~40 %) differences in the climatological mean distributions, seasonal cycle amplitude, and trends of the meridional and vertical winds. In the stratosphere there are similarly large (~50 %) differences in the magnitude, trends and seasonal cycle amplitude of the transformed Eulerian mean circulation and among various chemical and idealized tracers. At the same time, interannual variations in nearly all quantities are very well represented, compared to the underlying reanalyses. We show that the differences in magnitude, trends and seasonal cycle are not related to the use of different reanalysis products; rather, we show they are associated with how the simulations were implemented, by which we refer both to how the large-scale flow was prescribed and to biases in the underlying free-running models. In most cases these differences are shown to be as large or even larger than the differences exhibited by free-running simulations produced using the exact same models, which are also shown to be more dynamically consistent. Overall, our results suggest that care must be taken when using specified-dynamics simulations to examine the influence of large-scale dynamics on composition.

Fossil fuel and aerosol emissions have played important roles on climate over the Indian subcontinent over the last century. As the world transitions toward decarbonization in the next few decades, emissions pathways could have major impacts on India’s climate and people. Pathways for future emissions are highly uncertain, particularly at present as countries recover from COVID-19. This paper explores a multimodel ensemble of Earth system models leveraging potential global emissions pathways following COVID-19 and the consequences for India’s summertime (June–July–August–September) climate in the near- and long-term. We investigate specifically scenarios which envisage a fossil-based recovery, a strong renewable-based recovery and a moderate scenario in between the two. We find that near-term climate changes are dominated by natural climate variability, and thus likely independent of the emissions pathway. By 2050, pathway-induced spatial patterns in the seasonally-aggregated precipitation become clearer with a slight drying in the fossil-based scenario and wetting in the strong renewable scenario. Additionally, extreme temperature and precipitation events in India are expected to increase in magnitude and frequency regardless of the emissions scenario, though the spatial patterns of these changes as well as the extent of the change are pathway dependent. This study provides an important discussion on the impacts of emissions recover pathways following COVID-19 on India, a nation which is likely to be particularly susceptible to climate change over the coming decades.

The amount of dioxygen (O2) in the atmosphere may have varied from as little as 5 % to as much as 35 % during the Phanerozoic eon (54 Ma–present). These changes in the amount of O2 are large enough to have led to changes in atmospheric mass, which may alter the radiative budget of the atmosphere, leading to this mechanism being invoked to explain discrepancies between climate model simulations and proxy reconstructions of past climates. Here, we present the first fully 3-D numerical model simulations to investigate the climate impacts of changes in O2 under different climate states using the coupled atmosphere–ocean Hadley Centre Global Environmental Model version 3 (HadGEM3-AO) and Hadley Centre Coupled Model version 3 (HadCM3-BL) models. We show that simulations with an increase in O2 content result in increased global-mean surface air temperature under conditions of a pre-industrial Holocene climate state, in agreement with idealised 1-D and 2-D modelling studies. We demonstrate the mechanism behind the warming is complex and involves a trade-off between a number of factors. Increasing atmospheric O2 leads to a reduction in incident shortwave radiation at the Earth's surface due to Rayleigh scattering, a cooling effect. However, there is a competing warming effect due to an increase in the pressure broadening of greenhouse gas absorption lines and dynamical feedbacks, which alter the meridional heat transport of the ocean, warming polar regions and cooling tropical regions. Case studies from past climates are investigated using HadCM3-BL and show that, in the warmest climate states in the Maastrichtian (72.1–66.0 Ma), increasing oxygen may lead to a temperature decrease, as the equilibrium climate sensitivity is lower. For the Asselian (298.9–295.0 Ma), increasing oxygen content leads to a warmer global-mean surface temperature and reduced carbon storage on land, suggesting that high oxygen content may have been a contributing factor in preventing a “Snowball Earth” during this period of the early Permian. These climate model simulations reconcile the surface temperature response to oxygen content changes across the hierarchy of model complexity and highlight the broad range of Earth system feedbacks that need to be accounted for when considering the climate response to changes in atmospheric oxygen content.

The Southern Hemisphere (SH) zonal-mean circulation change in response to Antarctic ozone depletion is re-visited by examining a set of the latest model simulations archived for the Chemistry-Climate Model Initiative (CCMI) project. All models reasonably well reproduce Antarctic ozone depletion in the late 20th century. The related SH-summer circulation changes, such as a poleward intensification of westerly jet and a poleward expansion of the Hadley cell, are also well captured. All experiments exhibit quantitatively the same multi-model mean trend, irrespective of whether the ocean is coupled or prescribed. Results are also quantitatively similar to those derived from the Coupled Model Intercomparison Project phase 5 (CMIP5) high-top model simulations in which the stratospheric ozone is mostly prescribed with monthly- and zonally-averaged values. These results suggest that the ozone-hole-induced SH-summer circulation changes are robust across the models irrespective of the specific chemistry-atmosphere-ocean coupling.

Earth system models enable a broad range of climate interactions that physical climate models are unable to simulate. However, the extent to which adding Earth system components changes or improves the simulation of the physical climate is not well understood. Here we present a broad multivariate evaluation of the North Atlantic climate system in historical simulations of the UK Earth System Model (UKESM1) performed for CMIP6. In particular, we focus on the mean state and the decadal time scale evolution of important variables that span the North Atlantic climate system. In general, UKESM1 performs well and realistically simulates many aspects of the North Atlantic climate system. Like the physical version of the model, we find that changes in external forcing, and particularly aerosol forcing, are an important driver of multidecadal change in UKESM1, especially for Atlantic Multidecadal Variability and the Atlantic Meridional Overturning Circulation. However, many of the shortcomings identified are similar to common biases found in physical climate models, including the physical climate model that underpins UKESM1. For example, the summer jet is too weak and too far poleward; decadal variability in the winter jet is underestimated; intraseasonal stratospheric polar vortex variability is poorly represented; and Arctic sea ice is too thick. Forced shortwave changes may be also too strong in UKESM1, which, given the important role of historical aerosol forcing in shaping the evolution of the North Atlantic in UKESM1, motivates further investigation. Therefore, physical model development, alongside Earth system development, remains crucial in order to improve climate simulations. Plain Language Summary The North Atlantic climate system plays an important role in regulating Earth's climate, and variability within the Atlantic can have important impacts on society. However, we do not understand all the linkages between different parts of the North Atlantic. Furthermore, climate simulations, which are an essential tool for improving our understanding, have shortcomings that can affect their utility. New developments in Earth System climate simulations could remedy these shortcomings. However, we do not understand the extent to which the addition of complex Earth system developments have changed or improved the simulation of the physical climate. Therefore, in this paper, we present a multidisciplinary evaluation of the North Atlantic climate in simulations made with the UK's Earth System Model, UKESM1. We find that simulations made with UKESM1 capture many aspects of the North Atlantic climate and that human activities have a large impact on the North Atlantic in UKESM1. Nevertheless, we also highlight some shortcomings of the simulations, many of which are like those seen in physical climate simulations. Therefore, further development of both the physical and Earth system components is needed to improve climate simulations in the future. Key Points UKESM1 performs well across a range of variables and components of the North Atlantic climate system when compared with observations A range of shortcomings are still present in the simulations, however, with many shortcomings similar to those of the physical climate model Development of the physical model, alongside the Earth system components, is crucial for improved climate simulations