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Uncertainty in pre-industrial natural aerosol emissions is a major component of the overall uncertainty in the radiative forcing of climate. Improved characterisation of natural emissions and their radiative effects can therefore increase the accuracy of global climate model projections. Here we show that revised assumptions about pre-industrial fire activity result in significantly increased aerosol concentrations in the pre-industrial atmosphere. Revised global model simulations predict a 35% reduction in the calculated global mean cloud albedo forcing over the Industrial Era (1750–2000 CE) compared to estimates using emissions data from the Sixth Coupled Model Intercomparison Project. An estimated upper limit to pre-industrial fire emissions results in a much greater (91%) reduction in forcing. When compared to 26 other uncertain parameters or inputs in our model, pre-industrial fire emissions are by far the single largest source of uncertainty in pre-industrial aerosol concentrations, and hence in our understanding of the magnitude of the historical radiative forcing due to anthropogenic aerosol emissions. Several lines of evidence suggest that fire activity was much greater in the preindustrial era than currently assumed in climate models. Here the authors show that greater emission of aerosols from fires leads to a substantial reduction in the magnitude of aerosol radiative forcing over the Industrial Era.

The HadGEM2 earth system climate model was used to assess the impact of biomass burning on surface ozone concentrations over the Amazon forest and its impact on vegetation, under present-day climate conditions. Here we consider biomass burning emissions from wildfires, deforestation fires, agricultural forest burning, and residential and commercial combustion. Simulated surface ozone concentration is evaluated against observations taken at two sites in the Brazilian Amazon forest for years 2010 to 2012. The model is able to reproduce the observed diurnal cycle of surface ozone mixing ratio at the two sites, but overestimates the magnitude of the monthly averaged hourly measurements by 5–15 ppb for each available month at one of the sites. We vary biomass burning emissions over South America by ±20, 40, 60, 80 and 100% to quantify the modelled impact of biomass burning on surface ozone concentrations and ozone damage on vegetation productivity over the Amazon forest. We used the ozone damage scheme in the \"high\" sensitivity mode to give an upper limit for this effect. Decreasing South American biomass burning emissions by 100% (i.e. to zero) reduces surface ozone concentrations (by about 15 ppb during the biomass burning season) and suggests a 15% increase in monthly mean net primary productivity averaged over the Amazon forest, with local increases up to 60%. The simulated impact of ozone damage from present-day biomass burning on vegetation productivity is about 230 TgC yr−1. Taking into account that uncertainty in these estimates is substantial, this ozone damage impact over the Amazon forest is of the same order of magnitude as the release of carbon dioxide due to fire in South America; in effect it potentially doubles the impact of biomass burning on the carbon cycle.

We have reviewed the available scientific literature on how natural sources and the atmospheric fate of methane may be affected by future climate change. We discuss how processes governing methane wetland emissions, permafrost thawing, and destabilization of marine hydrates may affect the climate system. It is likely that methane wetland emissions will increase over the next century. Uncertainties arise from the temperature dependence of emissions and changes in the geographical distribution of wetland areas. Another major concern is the possible degradation or thaw of terrestrial permafrost due to climate change. The amount of carbon stored in permafrost, the rate at which it will thaw, and the ratio of methane to carbon dioxide emissions upon decomposition form the main uncertainties. Large amounts of methane are also stored in marine hydrates, and they could be responsible for large emissions in the future. The time scales for destabilization of marine hydrates are not well understood and are likely to be very long for hydrates found in deep sediments but much shorter for hydrates below shallow waters, such as in the Arctic Ocean. Uncertainties are dominated by the sizes and locations of the methane hydrate inventories, the time scales associated with heat penetration in the ocean and sediments, and the fate of methane released in the seawater. Overall, uncertainties are large, and it is difficult to be conclusive about the time scales and magnitudes of methane feedbacks, but significant increases in methane emissions are likely, and catastrophic emissions cannot be ruled out. We also identify gaps in our scientific knowledge and make recommendations for future research and development in the context of Earth system modeling.

We have implemented a process‐based isoprene emission model in the HadGEM2 Earth‐system model with coupled atmospheric chemistry in order to examine the feedback between isoprene emission and climate. Isoprene emissions and their impact on atmospheric chemistry and climate are estimated for preindustrial (1860–1869), present‐day (2000–2009), and future (2100–2109) climate conditions. The estimate of 460 TgC/yr for present‐day global total isoprene emission is consistent with previous estimates. Preindustrial isoprene emissions are estimated to be 26% higher than present‐day. Future isoprene emissions using the RCP8.5 scenario are similar to present‐day because increased emissions resulting from climate warming are countered by CO2 inhibition of isoprene emissions. The impact of biogenic isoprene emissions on the global O3 burden and CH4 lifetime is small but locally significant, and the impact of changes in isoprene emissions on atmospheric chemistry depends strongly on the state of climate and chemistry. Key Points Implementation of a process‐based isoprene emission scheme in Earth‐system model Feedback between isoprene emissions, atmospheric chemistry, and climate Impact of isoprene emissions on O3 and CH4 depends on climate and chemistry

Methane (CH4) is one of the most important trace gases in the atmosphere owing to its role as an exceedingly effective greenhouse gas and atmospheric pollutant. Better understanding of the global methane cycle and its interactions with the Earth system is therefore necessary for robust future projections of anthropogenic climate change and assessments of multi‐gas mitigation strategies. Here we present a newly developed methane emission‐driven Earth system model to simulate the global methane cycle fully interactively. We provide an evaluation of methane sources and sinks and a full‐cycle methane budget and its change over the historic period. We further evaluate the methane atmospheric abundance and lifetime against available observations. The new methane emission‐driven model simulates all the components of the methane cycle within observational uncertainty. We calculate a total present‐day (2000–2009 decadal average) methane source of 591 Tg(CH4) yr−1 with 197 Tg(CH4) yr−1 coming from wetlands. These sources are nearly balanced by the global methane sinks amounting to 580 Tg (CH4) yr−1; reaction of methane with the hydroxyl radical in the troposphere alone removes 525 Tg(CH4) yr−1. The imbalance between sources and sinks of 11 Tg(CH4) yr−1 represents the atmospheric methane growth rate and is in fairly good agreement with current best estimates of 5.8 Tg(CH4) yr−1 with a range of 4.9–6.6 Tg(CH4) yr−1. At present‐day the model shows a maximum systematic negative‐bias of approximately 200 ppb in the methane surface mole fraction. Plain Language Summary Methane is a very important greenhouse gas. The global methane cycle needs to be understood fully to accurately model the way methane affects climate change. We describe a new version of the UKESM1 Earth system model, UKESM1‐ems, that uses emissions of methane to drive the atmospheric chemistry. In case of emissions from global wetlands, such as bogs, swamps and tundra, the methane emissions are calculated by the model during runtime. Methane emissions react directly to changes in the modeled climate. UKESM1‐ems simulates the global cycle of methane from emissions via oxidation in the atmosphere to uptake at the surface more realistically. We also test the model against measurements from satellites and ground‐based stations to ensure the relevant processes in the model behave accurately. The comparison with observations shows that UKESM1‐ems performs well and represents an improvement in simulating important processes in climate and the Earth system. However, we also found that the methane concentration in the model is too low compared to observations for the period of the twentieth and early 21st century during which human activity, especially the use of fossil fuel, is dominating the methane cycle. Key Points A methane emission‐driven configuration of the UK community Earth system model UKESM1, UKESM1‐ems, has been developed In UKESM1‐ems global wetlands are interactively coupled to the atmosphere at every timestep via methane emissions The UKESM1‐ems performs well simulating the global methane cycle including feedbacks; the global budget compares well with observations

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, 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.

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 multimodel 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 (1CO/1NOx, 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 presentday 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.

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.

Diffuse light conditions can increase the efficiency of photosynthesis and carbon uptake by vegetation canopies. The diffuse fraction of photosynthetically active radiation (PAR) can be affected by either a change in the atmospheric aerosol burden and/or a change in cloudiness. During the dry season, a hotspot of biomass burning on the edges of the Amazon rainforest emits a complex mixture of aerosols and their precursors and climate-active trace gases (e.g. CO2, CH4, NOx). This creates potential for significant interactions between chemistry, aerosol, cloud, radiation and the biosphere across the Amazon region. The combined effects of biomass burning on the terrestrial carbon cycle for the present day are potentially large, yet poorly quantified. Here, we quantify such effects using the Met Office Hadley Centre Earth system model HadGEM2-ES, which provides a fully coupled framework with interactive aerosol, radiative transfer, dynamic vegetation, atmospheric chemistry and biogenic volatile organic compound emission components. Results show that for present day, defined as year 2000 climate, the overall net impact of biomass burning aerosols is to increase net primary productivity (NPP) by +80 to +105 TgC yr−1, or 1.9 % to 2.7 %, over the central Amazon Basin on annual mean. For the first time we show that this enhancement is the net result of multiple competing effects: an increase in diffuse light which stimulates photosynthetic activity in the shaded part of the canopy (+65 to +110 TgC yr−1), a reduction in the total amount of radiation (−52 to −105 TgC yr−1) which reduces photosynthesis and feedback from climate adjustments in response to the aerosol forcing which increases the efficiency of biochemical processes (+67 to +100 TgC yr−1). These results illustrate that despite a modest direct aerosol effect (the sum of the first two counteracting mechanisms), the overall net impact of biomass burning aerosols on vegetation is sizeable when indirect climate feedbacks are considered. We demonstrate that capturing the net impact of aerosols on vegetation should be assessed considering the system-wide behaviour.

Here we present a description of the UKCA StratTrop chemical mechanism, which is used in the UKESM1 Earth system model for CMIP6. The StratTrop chemical mechanism is a merger of previously well-evaluated tropospheric and stratospheric mechanisms, and we provide results from a series of bespoke integrations to assess the overall performance of the model.We find that the StratTrop scheme performs well when compared to a wide array of observations. The analysis we present here focuses on key components of atmospheric composition, namely the performance of the model to simulate ozone in the stratosphere and troposphere and constituents that are important for ozone in these regions. We find that the results obtained for tropospheric ozone and its budget terms from the use of the StratTrop mechanism are sensitive to the host model; simulations with the same chemical mechanism run in an earlier version of the MetUM host model show a range of sensitivity to emissions that the current model does not fall within.Whilst the general model performance is suitable for use in the UKESM1 CMIP6 integrations, we note some shortcomings in the scheme that future targeted studies will address.