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Elevated surface concentrations of ozone and fine particulate matter (PM 2.5 ) can lead to poor air quality and detrimental impacts on human health. These pollutants are also termed Near-Term Climate Forcers (NTCFs) as they can also influence the Earth's radiative balance on timescales shorter than long-lived greenhouse gases. Here we use the Earth system model, UKESM1, to simulate the change in surface ozone and PM 2.5 concentrations from different NTCF mitigation scenarios, conducted as part of the Aerosol and Chemistry Model Intercomparison Project (AerChemMIP). These are then combined with relative risk estimates and projected changes in population demographics, to estimate the mortality burden attributable to long-term exposure to ambient air pollution. Scenarios that involve the strong mitigation of air pollutant emissions yield large future benefits to human health (25%), particularly across Asia for black carbon (7%), when compared to the future reference pathway. However, if anthropogenic emissions follow the reference pathway, then impacts to human health worsen over South Asia in the short term (11%) and across Africa (20%) in the longer term. Future climate change impacts on air pollutants can offset some of the health benefits achieved by emission mitigation measures over Europe for PM 2.5 and East Asia for ozone. In addition, differences in the future chemical environment over regions are important considerations for mitigation measures to achieve the largest benefit to human health. Future policy measures to mitigate climate warming need to also consider the impact on air quality and human health across different regions to achieve the maximum co-benefits., Competing Interests: The authors declare no conflicts of interest relevant to this study., (© 2023 Crown copyright and The Authors. GeoHealth published by Wiley Periodicals LLC on behalf of American Geophysical Union. All Rights Reserved. This article is published with the permission of the Controller of HMSO and the King's Printer for Scotland.)

Atmospheric methane removal (e.g. in situ methane oxidation to carbon dioxide) may be needed to offset continued methane release and limit the global warming contribution of this potent greenhouse gas. Because mitigating most anthropogenic emissions of methane is uncertain this century, and sudden methane releases from the Arctic or elsewhere cannot be excluded, technologies for methane removal or oxidation may be required. Carbon dioxide removal has an increasingly well-established research agenda and technological foundation. No similar framework exists for methane removal. We believe that a research agenda for negative methane emissions-'removal' or atmospheric methane oxidation-is needed. We outline some considerations for such an agenda here, including a proposed Methane Removal Model Intercomparison Project (MR-MIP). This article is part of a discussion meeting issue 'Rising methane: is warming feeding warming? (part 1)'.

Mitigating climate change requires a diverse portfolio of technologies and approaches, including negative emissions or removal of greenhouse gases. Previous literature focuses primarily on carbon dioxide removal, but methane removal may be an important complement to future efforts. Methane removal has at least two key benefits: reducing temperature more rapidly than carbon dioxide removal and improving air quality by reducing surface ozone concentration. While some removal technologies are being developed, modelling of their impacts is limited. Here, we conduct the first simulations using a methane emissions-driven Earth System Model to quantify the climate and air quality co-benefits of methane removal, including different rates and timings of removal. We define a novel metric, the effective cumulative removal, and use it to show that each effective petagram of methane removed causes a mean global surface temperature reduction of 0.21 ± 0.04°C and a mean global surface ozone reduction of 1.0 ± 0.2 parts per billion. Our results demonstrate the effectiveness of methane removal in delaying warming thresholds and reducing peak temperatures, and also allow for direct comparisons between the impacts of methane and carbon dioxide removal that could guide future research and climate policy. This article is part of a discussion meeting issue 'Rising methane: is warming feeding warming? (part 1)'.

This study investigates changes in fine particulate matter (PM 2.5 ) concentration and air-quality index (AQI) in Asia using nine different Coupled Model Inter-Comparison Project 6 (CMIP6) climate model ensembles from historical and future scenarios under shared socioeconomic pathways (SSPs). The results indicated that the estimated present-day PM 2.5 concentrations were comparable to satellite-derived data. Overall, the PM 2.5 concentrations of the analyzed regions exceeded the WHO air-quality guidelines, particularly in East Asia and South Asia. In future SSP scenarios that consider the implementation of significant air-quality controls (SSP1-2.6, SSP5-8.5) and medium air-quality controls (SSP2-4.5), the annual PM 2.5 levels were predicted to substantially reduce (by 46% to around 66% of the present-day levels) in East Asia, resulting in a significant improvement in the AQI values in the mid-future. Conversely, weak air pollution controls considered in the SSP3-7.0 scenario resulted in poor AQI values in China and India. Moreover, a predicted increase in the percentage of aged populations (>65 years) in these regions, coupled with high AQI values, may increase the risk of premature deaths in the future. This study also examined the regional impact of PM 2.5 mitigations on downward shortwave energy and surface air temperature. Our results revealed that, although significant air pollution controls can reduce long-term exposure to PM 2.5 , it may also contribute to the warming of near- and mid-future climates.

Three Intergovernmental Panel on Climate Change (IPCC) Representative Concentration Pathways (RCPs) are used to simulate future ozone (O 3 ), nitrogen dioxide (NO 2 ), and fine particulate matter (PM 2.5 ) in the United Kingdom (UK) for the 2050s relative to the 2000s with an air quality model (AQUM) at a 12 km horizontal resolution. The present-day and future attributable fractions (AF) of mortality associated with long-term exposure to annual mean O 3 , NO 2 and PM 2.5 have accordingly been estimated for the first time for regions across England, Scotland and Wales. Across the three RCPs (RCP2.6, RCP6.0 and RCP8.5), simulated annual mean of the daily maximum 8-h mean (MDA8) O 3 concentrations increase compared to present-day, likely due to decreases in NO x (nitrogen oxides) emissions, leading to less titration of O 3 by NO. Annual mean NO 2 and PM 2.5 concentrations decrease under all RCPs for the 2050s, mostly driven by decreases in NO x and sulphur dioxide (SO 2 ) emissions, respectively. The AF of mortality associated with long-term exposure to annual mean MDA8 O 3 is estimated to increase in the future across all the regions and for all RCPs. Reductions in NO 2 and PM 2.5 concentrations lead to reductions in the AF estimated for future periods under all RCPs, for both pollutants. Total mortality burdens are also highly sensitive to future population projections. Accounting for population projections exacerbates differences in total UK-wide MDA8 O 3 -health burdens between present-day and future by up to a factor of ~3 but diminishes differences in NO 2 -health burdens. For PM 2.5 , accounting for future population projections results in additional UK-wide deaths brought forward compared to present-day under RCP2.6 and RCP6.0, even though the simulated PM 2.5 concentrations for the 2050s are estimated to decrease. Thus, these results highlight the sensitivity of future health burdens in the UK to future trends in atmospheric emissions over the UK as well as future population projections., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2021 Elsevier B.V. All rights reserved.)

We have derived values of the Ultraviolet Index (UVI) at solar noon using the Tropospheric Ultraviolet Model (TUV) driven by ozone, temperature and aerosol fields from climate simulations of the first phase of the Chemistry-Climate Model Initiative (CCMI-1). Since clouds remain one of the largest uncertainties in climate projections, we simulated only the clear-sky UVI. We compared the modelled UVI climatologies against present-day climatological values of UVI derived from both satellite data (the OMI-Aura OMUVBd product) and ground-based measurements (from the NDACC network). Depending on the region, relative differences between the UVI obtained from CCMI/TUV calculations and the ground-based measurements ranged between -5.9% and 10.6%. We then calculated the UVI evolution throughout the 21st century for the four Representative Concentration Pathways (RCPs 2.6, 4.5, 6.0 and 8.5). Compared to 1960s values, we found an average increase in the UVI in 2100 (of 2-4%) in the tropical belt (30°N-30°S). For the mid-latitudes, we observed a 1.8 to 3.4 % increase in the Southern Hemisphere for RCP 2.6, 4.5 and 6.0, and found a 2.3% decrease in RCP 8.5. Higher increases in UVI are projected in the Northern Hemisphere except for RCP 8.5. At high latitudes, ozone recovery is well identified and induces a complete return of mean UVI levels to 1960 values for RCP 8.5 in the Southern Hemisphere. In the Northern Hemisphere, UVI levels in 2100 are higher by 0.5 to 5.5% for RCP 2.6, 4.5 and 6.0 and they are lower by 7.9% for RCP 8.5. We analysed the impacts of greenhouse gases (GHGs) and ozone-depleting substances (ODSs) on UVI from 1960 by comparing CCMI sensitivity simulations (1960-2100) with fixed GHGs or ODSs at their respective 1960 levels. As expected with ODS fixed at their 1960 levels, there is no large decrease in ozone levels and consequently no sudden increase in UVI levels. With fixed GHG, we observed a delayed return of ozone to 1960 values, with a corresponding pattern of change observed on UVI, and looking at the UVI difference between 2090s values and 1960s values, we found an 8 % increase in the tropical belt during the summer of each hemisphere. Finally we show that, while in the Southern Hemisphere the UVI is mainly driven by total ozone column, in the Northern Hemisphere both total ozone column and aerosol optical depth drive UVI levels, with aerosol optical depth having twice as much influence on the UVI as total ozone column does.

Previous multi-model intercomparisons have shown that chemistry-climate models exhibit significant biases in tropospheric ozone compared with observations. We investigate annual-mean tropospheric column ozone in 15 models participating in the SPARC/IGAC (Stratosphere-troposphere Processes and their Role in Climate/International Global Atmospheric Chemistry) Chemistry-Climate Model Initiative (CCMI). These models exhibit a positive bias, on average, of up to 40-50% in the Northern Hemisphere compared with observations derived from the Ozone Monitoring Instrument and Microwave Limb Sounder (OMI/MLS), and a negative bias of up to ~30% in the Southern Hemisphere. SOCOLv3.0 (version 3 of the Solar-Climate Ozone Links CCM), which participated in CCMI, simulates global-mean tropospheric ozone columns of 40.2 DU - approximately 33% larger than the CCMI multi-model mean. Here we introduce an updated version of SOCOLv3.0, "SOCOLv3.1", which includes an improved treatment of ozone sink processes, and results in a reduction in the tropospheric column ozone bias of up to 8 DU, mostly due to the inclusion of N 2 O 5 hydrolysis on tropospheric aerosols. As a result of these developments, tropospheric column ozone amounts simulated by SOCOLv3.1 are comparable with several other CCMI models. We apply Gaussian process emulation and sensitivity analysis to understand the remaining ozone bias in SOCOLv3.1. This shows that ozone precursors (nitrogen oxides (NO x ), carbon monoxide, methane and other volatile organic compounds) are responsible for more than 90% of the variance in tropospheric ozone. However, it may not be the emissions inventories themselves that result in the bias, but how the emissions are handled in SOCOLv3.1, and we discuss this in the wider context of the other CCMI models. Given that the emissions data set to be used for phase 6 of the Coupled Model Intercomparison Project includes approximately 20% more NO x than the data set used for CCMI, further work is urgently needed to address the challenges of simulating sub-grid processes of importance to tropospheric ozone in the current generation of chemistry-climate models.

Major stratospheric sudden warmings (SSWs) are the largest instance of wintertime variability in the Arctic stratosphere. Due to their relevance for the troposphere-stratosphere system, several previous studies have focused on their potential response to anthropogenic forcings. However, a wide range of results have been reported, from a future increase in the frequency of SSWs to a decrease. Several factors might explain these contradictory results, notably the use of different metrics for the identification of SSWs, and the impact of large climatological biases in single-model studies. Here we revisit the question of future SSWs changes, using an identical set of metrics applied consistently across 12 different models participating in the Chemistry Climate Model Initiative. From analyzing future integrations we find no statistically significant change in the frequency of SSWs over the 21 st century, irrespective of the metric used for the identification of SSWs. Changes in other SSWs characteristics, such as their duration and the tropospheric forcing, are also assessed: again, we find no evidence of future changes over the 21 st century.

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.

This review examines the current literature on the effects of future emissions and climate change on particulate matter (PM) and O 3 air quality and on the consequent health impacts, with a focus on Europe. There is considerable literature on the effects of climate change on O 3 but fewer studies on the effects of climate change on PM concentrations. Under the latest Intergovernmental Panel on Climate Change (IPCC) 5th assessment report (AR5) Representative Concentration Pathways (RCPs), background O 3 entering Europe is expected to decrease under most scenarios due to higher water vapour concentrations in a warmer climate. However, under the extreme pathway RCP8.5 higher (more than double) methane (CH 4 ) abundances lead to increases in background O 3 that offset the O 3 decrease due to climate change especially for the 2100 period. Regionally, in polluted areas with high levels of nitrogen oxides (NO x ), elevated surface temperatures and humidities yield increases in surface O 3 - termed the O 3 climate penalty - especially in southern Europe. The O 3 response is larger for metrics that represent the higher end of the O 3 distribution, such as daily maximum O 3 . Future changes in PM concentrations due to climate change are much less certain, although several recent studies also suggest a PM climate penalty due to high temperatures and humidity and reduced precipitation in northern mid-latitude land regions in 2100.A larger number of studies have examined both future climate and emissions changes under the RCP scenarios. Under these pathways the impact of emission changes on air quality out to the 2050s will be larger than that due to climate change, because of large reductions in emissions of O 3 and PM pollutant precursor emissions and the more limited climate change response itself. Climate change will also affect climate extreme events such as heatwaves. Air pollution episodes are associated with stagnation events and sometimes heat waves. Air quality during the 2003 heatwave over Europe has been examined in numerous studies and mechanisms for enhancing O 3 have been identified.There are few studies on health effects associated with climate change impacts alone on air quality, but these report higher O 3 -related health burdens in polluted populated regions and greater PM 2.5 health burdens in these emission regions. Studies that examine the combined impacts of climate change and anthropogenic emissions change under the RCP scenarios report reductions in global and European premature O 3 -respiratory related and PM mortalities arising from the large decreases in precursor emissions. Under RCP 8.5 the large increase in CH 4 leads to global and European excess O 3 -respiratory related mortalities in 2100. For future health effects, besides uncertainty in future O 3 and particularly PM concentrations, there is also uncertainty in risk estimates such as effect modification by temperature on pollutant-response relationships and potential future adaptation that would alter exposure risk.

This corrects the article DOI: 10.1038/nature22974.

Aerosols have a potentially large effect on climate, particularly through their interactions with clouds, but the magnitude of this effect is highly uncertain. Large volcanic eruptions produce sulfur dioxide, which in turn produces aerosols; these eruptions thus represent a natural experiment through which to quantify aerosol-cloud interactions. Here we show that the massive 2014-2015 fissure eruption in Holuhraun, Iceland, reduced the size of liquid cloud droplets-consistent with expectations-but had no discernible effect on other cloud properties. The reduction in droplet size led to cloud brightening and global-mean radiative forcing of around -0.2 watts per square metre for September to October 2014. Changes in cloud amount or cloud liquid water path, however, were undetectable, indicating that these indirect effects, and cloud systems in general, are well buffered against aerosol changes. This result will reduce uncertainties in future climate projections, because we are now able to reject results from climate models with an excessive liquid-water-path response.

Background: Estimating the long-term health impact of air pollution in a spatio-temporal ecological study requires representative concentrations of air pollutants to be constructed for each geographical unit and time period. Averaging concentrations in space and time is commonly carried out, but little is known about how robust the estimated health effects are to different aggregation functions. A second under researched question is what impact air pollution is likely to have in the future., Methods: We conducted a study for England between 2007 and 2011, investigating the relationship between respiratory hospital admissions and different pollutants: nitrogen dioxide (NO 2 ); ozone (O 3 ); particulate matter, the latter including particles with an aerodynamic diameter less than 2.5 micrometers (PM 2.5 ), and less than 10 micrometers (PM 10 ); and sulphur dioxide (SO 2 ). Bayesian Poisson regression models accounting for localised spatio-temporal autocorrelation were used to estimate the relative risks (RRs) of pollution on disease risk, and for each pollutant four representative concentrations were constructed using combinations of spatial and temporal averages and maximums. The estimated RRs were then used to make projections of the numbers of likely respiratory hospital admissions in the 2050s attributable to air pollution, based on emission projections from a number of Representative Concentration Pathways (RCP)., Results: NO 2 exhibited the largest association with respiratory hospital admissions out of the pollutants considered, with estimated increased risks of between 0.9 and 1.6% for a one standard deviation increase in concentrations. In the future the projected numbers of respiratory hospital admissions attributable to NO 2 in the 2050s are lower than present day rates under 3 Representative Concentration Pathways (RCPs): 2.6, 6.0, and 8.5, which is due to projected reductions in future NO 2 emissions and concentrations., Conclusions: NO 2 concentrations exhibit consistent substantial present-day health effects regardless of how a representative concentration is constructed in space and time. Thus as concentrations are predicted to remain above limits set by European Union Legislation until the 2030s in parts of urban England, it will remain a substantial health risk for some time.

Atmospheric methane (CH 4 ) varied with climate during the Quaternary, rising from a concentration of 375 p.p.b.v. during the last glacial maximum (LGM) 21,000 years ago, to 680 p.p.b.v. at the beginning of the industrial revolution. However, the causes of this increase remain unclear; proposed hypotheses rely on fluctuations in either the magnitude of CH 4 sources or CH 4 atmospheric lifetime, or both. Here we use an Earth System model to provide a comprehensive assessment of these competing hypotheses, including estimates of uncertainty. We show that in this model, the global LGM CH 4 source was reduced by 28-46%, and the lifetime increased by 2-8%, with a best-estimate LGM CH 4 concentration of 463-480 p.p.b.v. Simulating the observed LGM concentration requires a 46-49% reduction in sources, indicating that we cannot reconcile the observed amplitude. This highlights the need for better understanding of the effects of low CO 2 and cooler climate on wetlands and other natural CH 4 sources.

Emissions of air pollutants and their precursors determine regional air quality and can alter climate. Climate change can perturb the long-range transport, chemical processing, and local meteorology that influence air pollution. We review the implications of projected changes in methane (CH(4)), ozone precursors (O(3)), and aerosols for climate (expressed in terms of the radiative forcing metric or changes in global surface temperature) and hemispheric-to-continental scale air quality. Reducing the O(3) precursor CH(4) would slow near-term warming by decreasing both CH(4) and tropospheric O(3). Uncertainty remains as to the net climate forcing from anthropogenic nitrogen oxide (NO(x)) emissions, which increase tropospheric O(3) (warming) but also increase aerosols and decrease CH(4) (both cooling). Anthropogenic emissions of carbon monoxide (CO) and non-CH(4) volatile organic compounds (NMVOC) warm by increasing both O(3) and CH(4). Radiative impacts from secondary organic aerosols (SOA) are poorly understood. Black carbon emission controls, by reducing the absorption of sunlight in the atmosphere and on snow and ice, have the potential to slow near-term warming, but uncertainties in coincident emissions of reflective (cooling) aerosols and poorly constrained cloud indirect effects confound robust estimates of net climate impacts. Reducing sulfate and nitrate aerosols would improve air quality and lessen interference with the hydrologic cycle, but lead to warming. A holistic and balanced view is thus needed to assess how air pollution controls influence climate; a first step towards this goal involves estimating net climate impacts from individual emission sectors. Modeling and observational analyses suggest a warming climate degrades air quality (increasing surface O(3) and particulate matter) in many populated regions, including during pollution episodes. Prior Intergovernmental Panel on Climate Change (IPCC) scenarios (SRES) allowed unconstrained growth, whereas the Representative Concentration Pathway (RCP) scenarios assume uniformly an aggressive reduction, of air pollutant emissions. New estimates from the current generation of chemistry-climate models with RCP emissions thus project improved air quality over the next century relative to those using the IPCC SRES scenarios. These two sets of projections likely bracket possible futures. We find that uncertainty in emission-driven changes in air quality is generally greater than uncertainty in climate-driven changes. Confidence in air quality projections is limited by the reliability of anthropogenic emission trajectories and the uncertainties in regional climate responses, feedbacks with the terrestrial biosphere, and oxidation pathways affecting O(3) and SOA.