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Estimates of aviation effective radiative forcing (ERF) indicate that contrail cirrus is currently its largest contributor, although with a substantial associated uncertainty of ∼ 70 %. Here, we implement the contrail parameterisation developed for the Community Atmosphere Model (CAM) in the UK Met Office Unified Model (UM), allowing us to compare, for the first time, the impact of key features of the host climate model on contrail cirrus ERF. We find that differences in background humidity between the models result in the UM-simulated contrail fractions being 2 to 3 times larger than in CAM. Additionally, the models show contrasting responses in overall global cloud fraction, with contrails increasing the total cloud fraction in the UM and decreasing it in CAM. Differences in the complexity of the cloud microphysics schemes lead to significant differences in simulated changes to cloud ice water content due to aviation. After compensating for the unrealistically low contrail optical depth in the UM, we estimate the 2018 contrail cirrus ERF to be 40.8 mW m−2 in the UM, compared to 60.1 mW m−2 in CAM. These values highlight the substantial uncertainty in contrail cirrus ERF due to differences in microphysics and radiation schemes between the two models. We also find a factor-of-8 uncertainty in contrail cirrus ERF due to existing uncertainty in contrail cirrus optical depth. Future research should focus on better representing microphysical and radiative contrail characteristics in climate models and on improved observational constraints.

Using state-of-the-art satellite ozone profile products, and a chemical transport model, we provide an updated estimate of the tropospheric ozone radiative effect (TO3RE) and observational constraint on its variability over the decade 2008–2017. Previous studies have shown the short-term (i.e. a few years) globally weighted average TO3RE to be 1.17 ± 0.03 W m−2. However, from our analysis, using decadal (2008–2017) ozone profile datasets from the Infrared Atmospheric Sounding Interferometer, average TO3RE ranges between 1.21 and 1.26 W m−2. Over this decade, the modelled and observational TO3RE linear trends show a negligible change (e.g. ± 0.1 % yr−1). Two model sensitivity experiments fixing emissions and meteorology to 1 year (i.e. start year – 2008) show that temporal changes in ozone precursor emissions (increasing contribution) and meteorological factors (decreasing contribution) have counteracting tendencies, leading to a negligible globally weighted average TO3RE trend.

Cirrus clouds play an important role in the radiation budget of the Earth; nonetheless, the radiative effect of ultra-thin cirrus clouds in the tropopause region and in the lowermost stratosphere remains poorly constrained. These clouds have a small vertical extent and optical depth and are frequently neither observed even by sensitive sensors nor considered in climate model simulations. In addition, their short-wave (cooling) and long-wave (warming) radiative effects are often in approximate balance, and their net effect strongly depends on the shape and size of the cirrus particles. However, the CRyogenic Infrared Spectrometers and Telescopes for the Atmosphere instrument (CRISTA-2) allows ultra-thin cirrus clouds to be detected. Here we use CRISTA-2 observations in summer 1997 in the Northern Hemisphere midlatitudes together with the Suite Of Community RAdiative Transfer codes based on Edwards and Slingo (SOCRATES) radiative transfer model to calculate the radiative effect of observed ultra-thin cirrus. Using sensitivity simulations with different ice effective particle size and shape, we provide an estimate of the uncertainty in the radiative effect of ultra-thin cirrus in the extratropical lowermost stratosphere and tropopause region during summer and – by extrapolation of the summer results – for winter. Cloud top height and ice water content are based on CRISTA-2 measurements, while the cloud vertical thickness was predefined to be 0.5 or 2 km. Our results indicate that if the ice crystals of these thin cirrus clouds are assumed to be spherical, their net cloud radiative effect is generally positive (warming). In contrast, assuming aggregates or a hexagonal shape, their net radiative effect is generally negative (cooling) during summer months and very likely positive (warming) during winter. The radiative effect is in the order of ±(0.1–0.01) W m−2 for a realistic global cloud coverage of 10 %, similar to the magnitude of the contrail cirrus radiative forcing (of ∼ 0.1 W m−2). The radiative effect is also dependent on the cloud vertical extent and consequently the optically thickness and effective radius of the particle size distribution (e.g. effective radius increase from 5 to 30 µm results in a factor ∼ 6 smaller long- and short-wave effects, respectively). The properties of ultra-thin cirrus clouds in the lowermost stratosphere and tropopause region need to be better observed, and ultra-thin cirrus clouds need to be evaluated in climate model simulations.

The rapid melting of glaciers in the Hindu Kush Himalayas (HKH) during recent decades poses an alarming threat to water security for larger parts of Asia. If this melting persists, the entirety of the Himalayan glaciers are estimated to disappear by end of the 21st century. Here, we assess the influence of the spring 2020 COVID-19 lockdown on the HKH, demonstrating the potential benefits of a strict emission reduction roadmap. Chemistry–climate model simulations, supported by satellite and ground measurements, show that lower levels of gas and aerosol pollution during lockdown led to changes in meteorology and to a reduction in black carbon in snow (2 %–14 %) and thus a reduction in snowmelt (10 %–40 %). This caused increases in snow cover (6 %–12 %) and mass (2 %–20 %) and a decrease in runoff (5 %–55 %) over the HKH and Tibetan Plateau, ultimately leading to an enhanced snow-equivalent water (2 %–55 %). We emphasize the necessity for immediate anthropogenic pollution reductions to address the hydro-climatic threat to billions of people in southern Asia.

Atmospheric concentrations of South Asian anthropogenic aerosols and their transport play a key role in the regional hydrological cycle. Here, we use the ECHAM6-HAMMOZ chemistry–climate model to show the structure and implications of the transport pathways of these aerosols during spring (March–May). Our simulations indicate that large amounts of anthropogenic aerosols are transported from South Asia to the northern Indian Ocean and western Pacific. These aerosols are then lifted into the upper troposphere and lower stratosphere (UTLS) by the ascending branch of the Hadley circulation, where they enter the westerly jet. They are further transported to the Southern Hemisphere (∼15–30∘ S) and downward (320–340 K) via westerly ducts over the tropical Atlantic (5∘ S–5∘ N, 10–40∘ W) and Pacific (5∘ S–5∘ N, 95–140∘ E). The carbonaceous aerosols are also transported to the Arctic, leading to local heating (0.08–0.3 K per month, an increase by 10 %–60 %). The presence of anthropogenic aerosols causes a negative radiative forcing (RF) at the top of the atmosphere (TOA) (−0.90 ± 0.089 W m−2) and surface (−5.87 ± 0.31 W m−2) and atmospheric warming (+4.96 ± 0.24 W m−2) over South Asia (60–90∘ E, 8–23∘ N), except over the Indo-Gangetic Plain (75–83∘ E, 23–30∘ N), where RF at the TOA is positive (+1.27 ± 0.16 W m−2) due to large concentrations of absorbing aerosols. The carbonaceous aerosols lead to in-atmospheric heating along the aerosol column extending from the boundary layer to the upper troposphere (0.1 to 0.4 K per month, increase by 4 %–60 %) and in the lower stratosphere at 40–90∘ N (0.02 to 0.3 K per month, increase by 10 %–60 %). The increase in tropospheric heating due to aerosols results in an increase in water vapor concentrations, which are then transported from the northern Indian Ocean–western Pacific to the UTLS over 45–45∘ N (increasing water vapor by 1 %–10 %).

Tropospheric ozone concentrations are sensitive to natural emissions of precursor compounds. In contrast to existing assumptions, recent evidence indicates that terrestrial vegetation emissions in the pre-industrial era were larger than in the present day. We use a chemical transport model and a radiative transfer model to show that revised inventories of pre-industrial fire and biogenic emissions lead to an increase in simulated pre-industrial ozone concentrations, decreasing the estimated pre-industrial to present-day tropospheric ozone radiative forcing by up to 34 % (0.38 to 0.25 W m−2). We find that this change is sensitive to employing biomass burning and biogenic emissions inventories based on matching vegetation patterns, as the co-location of emission sources enhances the effect on ozone formation. Our forcing estimates are at the lower end of existing uncertainty range estimates (0.2–0.6 W m−2), without accounting for other sources of uncertainty. Thus, future work should focus on reassessing the uncertainty range of tropospheric ozone radiative forcing.

Convective transport plays a key role in aerosol enhancement in the upper troposphere and lower stratosphere (UTLS) over the Asian monsoon region where low-level convective instability persists throughout the year. We use the state-of-the-art ECHAM6–HAMMOZ global chemistry–climate model to investigate the seasonal transport of anthropogenic Asian sulfate aerosols and their impact on the UTLS. Sensitivity simulations for SO2 emission perturbation over India (48 % increase) and China (70 % decrease) are performed based on the Ozone Monitoring Instrument (OMI) satellite-observed trend, rising over India by ∼4.8 % per year and decreasing over China by ∼7.0 % per year during 2006–2017. The enhanced Indian emissions result in an increase in aerosol optical depth (AOD) loading in the UTLS by 0.61 to 4.17 % over India. These aerosols are transported to the Arctic during all seasons by the lower branch of the Brewer–Dobson circulation enhancing AOD by 0.017 % to 4.8 %. Interestingly, a reduction in SO2 emission over China inhibits the transport of Indian sulfate aerosols to the Arctic in summer-monsoon and post-monsoon seasons due to subsidence over northern India. The region of sulfate aerosol enhancement shows significant warming in the UTLS over northern India, south China (0.2±0.15 to 0.8±0.72 K) and the Arctic (∼1±0.62 to 1.6±1.07 K). The estimated seasonal mean direct radiative forcing at the top of the atmosphere (TOA) induced by the increase in Indian SO2 emission is −0.2 to −1.5 W m−2 over northern India. The Chinese SO2 emission reduction leads to a positive radiative forcing of ∼0.6 to 6 W m−2 over China. The decrease in vertical velocity and the associated enhanced stability of the upper troposphere in response to increased Indian SO2 emissions will likely decrease rainfall over India.

The interannual variability of the greenhouse gases methane (CH4) and tropospheric ozone (O3) is largely driven by natural variations in global emissions and meteorology. The El Niño–Southern Oscillation (ENSO) is known to influence fire occurrence, wetland emission and atmospheric circulation, affecting sources and sinks of CH4 and tropospheric O3, but there are still important uncertainties associated with the exact mechanism and magnitude of this effect. Here we use a modelling approach to investigate how fires and meteorology control the interannual variability of global carbon monoxide (CO), CH4 and O3 concentrations, particularly during large El Niño events. Using a three-dimensional chemical transport model (TOMCAT) coupled to a sophisticated aerosol microphysics scheme (GLOMAP) we simulate changes to CO, hydroxyl radical (OH) and O3 for the period 1997–2014. We then use an offline radiative transfer model to quantify the climate impact of changes to atmospheric composition as a result of specific drivers. During the El Niño event of 1997–1998, there were increased emissions from biomass burning globally, causing global CO concentrations to increase by more than 40 %. This resulted in decreased global mass-weighted tropospheric OH concentrations of up to 9 % and a consequent 4 % increase in the CH4 atmospheric lifetime. The change in CH4 lifetime led to a 7.5 ppb yr−1 increase in the global mean CH4 growth rate in 1998. Therefore, biomass burning emission of CO could account for 72 % of the total effect of fire emissions on CH4 growth rate in 1998. Our simulations indicate that variations in fire emissions and meteorology associated with El Niño have opposing impacts on tropospheric O3 burden. El Niño-related changes in atmospheric transport and humidity decrease global tropospheric O3 concentrations leading to a −0.03 W m−2 change in the O3 radiative effect (RE). However, enhanced fire emission of precursors such as nitrogen oxides (NOx) and CO increase O3 and lead to an O3 RE of 0.03 W m−2. While globally the two mechanisms nearly cancel out, causing only a small change in global mean O3 RE, the regional changes are large – up to −0.33 W m−2 with potentially important consequences for atmospheric heating and dynamics.

The highly vibrant Asian summer monsoon (ASM) anticyclone plays an important role in efficient transport of Asian tropospheric air masses to the extratropical upper troposphere and lower stratosphere (UTLS). In this paper, we demonstrate long-range transport of Asian trace gases via eddy-shedding events using MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) satellite observations, ERA-Interim reanalysis data and the ECHAM5–HAMMOZ global chemistry-climate model. Model simulations and observations consistently show that Asian boundary layer trace gases are lifted to UTLS altitudes in the monsoon anticyclone and are further transported horizontally eastward and westward by eddies detached from the anticyclone. We present an event of eddy shedding during 1–8 July 2003 and discuss a 1995–2016 climatology of eddy-shedding events. Our analysis indicates that eddies detached from the anticyclone contribute to the transport of Asian trace gases away from the Asian region to the western Pacific (20–30° N, 120–150° E) and western Africa (20–30° N, 0–30° E). Over the last two decades, the estimated frequency of occurrence of eddy-shedding events is ∼ 68 % towards western Africa and ∼ 25 % towards the western Pacific.Model sensitivity experiments considering a 10 % reduction in Asian emissions of non-methane volatile organic compounds (NMVOCs) and nitrogen oxides (NOx) were performed with ECHAM5–HAMMOZ to understand the impact of Asian emissions on the UTLS. The model simulations show that transport of Asian emissions due to eddy shedding significantly affects the chemical composition of the upper troposphere ( ∼ 100–400 hPa) and lower stratosphere ( ∼ 100–80 hPa) over western Africa and the western Pacific. The 10 % reduction of NMVOCs and NOx Asian emissions leads to decreases in peroxyacetyl nitrate (PAN) (2 %–10 % near 200–80 hPa), ozone (1 %–4.5 % near ∼ 150 hPa) and ozone heating rates (0.001–0.004 K day−1 near 300–150 hPa) in the upper troposphere over western Africa and the western Pacific.

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.

Over the 21st century changes in both tropospheric and stratospheric ozone are likely to have important consequences for the Earth's radiative balance. In this study, we investigate the radiative forcing from future ozone changes using the Community Earth System Model (CESM1), with the Whole Atmosphere Community Climate Model (WACCM), and including fully coupled radiation and chemistry schemes. Using year 2100 conditions from the Representative Concentration Pathway 8.5 (RCP8.5) scenario, we quantify the individual contributions to ozone radiative forcing of (1) climate change, (2) reduced concentrations of ozone depleting substances (ODSs), and (3) methane increases. We calculate future ozone radiative forcings and their standard error (SE; associated with inter-annual variability of ozone) relative to year 2000 of (1) 33 ± 104 m Wm−2, (2) 163 ± 109 m Wm−2, and (3) 238 ± 113 m Wm−2 due to climate change, ODSs, and methane, respectively. Our best estimate of net ozone forcing in this set of simulations is 430 ± 130 m Wm−2 relative to year 2000 and 760 ± 230 m Wm−2 relative to year 1750, with the 95 % confidence interval given by ±30 %. We find that the overall long-term tropospheric ozone forcing from methane chemistry–climate feedbacks related to OH and methane lifetime is relatively small (46 m Wm−2). Ozone radiative forcing associated with climate change and stratospheric ozone recovery are robust with regard to background climate conditions, even though the ozone response is sensitive to both changes in atmospheric composition and climate. Changes in stratospheric-produced ozone account for ∼ 50 % of the overall radiative forcing for the 2000–2100 period in this set of simulations, highlighting the key role of the stratosphere in determining future ozone radiative forcing.

The climate impacts of deforestation due to changes in biogenic volatile organic compound emissions, which act as short-lived climate forcers (SLCFs), are poorly understood. Here the authors show that including the impact SLCFs increases the projected warming associated with idealised deforestation scenarios.

The Asian summer monsoon (ASM) anticyclone is the most pronounced circulation pattern in the upper troposphere and lower stratosphere (UTLS) during northern hemispheric summer. ASM convection plays an important role in efficient vertical transport from the surface to the upper-level anticyclone. In this paper we investigate the potential impact of enhanced anthropogenic nitrogen oxide (NOx) emissions on the distribution of ozone in the UTLS using the fully coupled aerosol–chemistry–climate model, ECHAM5-HAMMOZ. Ozone in the UTLS is influenced both by the convective uplift of ozone precursors and by the uplift of enhanced-NOx-induced tropospheric ozone anomalies. We performed anthropogenic NOx emission sensitivity experiments over India and China. In these simulations, covering the years 2000–2010, anthropogenic NOx emissions have been increased by 38 % over India and by 73 % over China with respect to the emission base year 2000. These emission increases are comparable to the observed linear trends of 3.8 % per year over India and 7.3 % per year over China during the period 2000 to 2010. Enhanced NOx emissions over India by 38 % and China by 73 % increase the ozone radiative forcing in the ASM anticyclone (15–40° N, 60–120° E) by 16.3 and 78.5 mW m−2 respectively. These elevated NOx emissions produce significant warming over the Tibetan Plateau and increase precipitation over India due to a strengthening of the monsoon Hadley circulation. However, increase in NOx emissions over India by 73 % (similar to the observed increase over China) results in large ozone production over the Indo-Gangetic Plain and Tibetan Plateau. The higher ozone concentrations, in turn, induce a reversed monsoon Hadley circulation and negative precipitation anomalies over India. The associated subsidence suppresses vertical transport of NOx and ozone into the ASM anticyclone.

Aviation emissions impact both air quality and climate. Using a coupled tropospheric chemistry-aerosol microphysics model we investigate the effects of varying aviation fuel sulfur content (FSC) on premature mortality from long-term exposure to aviation-sourced PM2.5 (particulate matter with a dry diameter of 2 aviation emissions with a typical FSC of 600 ppm result in ∼ 3600 [95 % CI: 1310–5890] annual premature mortalities globally due to increases in cases of cardiopulmonary disease and lung cancer, resulting from increased surface PM2.5 concentrations. We quantify the global annual mean combined radiative effect (REcomb) of non-CO2 aviation emissions as −13.3 mW m−2; from increases in aerosols (direct radiative effect and cloud albedo effect) and tropospheric ozone. Ultra-low sulfur jet fuel (ULSJ; FSC = 15 ppm) has been proposed as an option to reduce the adverse health impacts of aviation-induced PM2.5. We calculate that swapping the global aviation fleet to ULSJ fuel would reduce the global aviation-induced mortality rate by ∼ 620 [95 % CI: 230–1020] mortalities a−1 and increase REcomb by +7.0 mW m−2. We explore the impact of varying aviation FSC between 0 and 6000 ppm. Increasing FSC increases aviation-induced mortality, while enhancing climate cooling through increasing the aerosol cloud albedo effect (CAE). We explore the relationship between the injection altitude of aviation emissions and the resulting climate and air quality impacts. Compared to the standard aviation emissions distribution, releasing aviation emissions at the ground increases global aviation-induced mortality and produces a net warming effect, primarily through a reduced CAE. Aviation emissions injected at the surface are 5 times less effective at forming cloud condensation nuclei, reducing the aviation-induced CAE by a factor of 10. Applying high FSCs at aviation cruise altitudes combined with ULSJ fuel at lower altitudes results in reduced aviation-induced mortality and increased negative RE compared to the baseline aviation scenario.

Combustion of fuels in the residential sector for cooking and heating results in the emission of aerosol and aerosol precursors impacting air quality, human health, and climate. Residential emissions are dominated by the combustion of solid fuels. We use a global aerosol microphysics model to simulate the impact of residential fuel combustion on atmospheric aerosol for the year 2000. The model underestimates black carbon (BC) and organic carbon (OC) mass concentrations observed over Asia, Eastern Europe, and Africa, with better prediction when carbonaceous emissions from the residential sector are doubled. Observed seasonal variability of BC and OC concentrations are better simulated when residential emissions include a seasonal cycle. The largest contributions of residential emissions to annual surface mean particulate matter (PM2.5) concentrations are simulated for East Asia, South Asia, and Eastern Europe. We use a concentration response function to estimate the human health impact due to long-term exposure to ambient PM2.5 from residential emissions. We estimate global annual excess adult (> 30 years of age) premature mortality (due to both cardiopulmonary disease and lung cancer) to be 308 000 (113 300–497 000, 5th to 95th percentile uncertainty range) for monthly varying residential emissions and 517 000 (192 000–827 000) when residential carbonaceous emissions are doubled. Mortality due to residential emissions is greatest in Asia, with China and India accounting for 50 % of simulated global excess mortality. Using an offline radiative transfer model we estimate that residential emissions exert a global annual mean direct radiative effect between −66 and +21 mW m−2, with sensitivity to the residential emission flux and the assumed ratio of BC, OC, and SO2 emissions. Residential emissions exert a global annual mean first aerosol indirect effect of between −52 and −16 mW m−2, which is sensitive to the assumed size distribution of carbonaceous emissions. Overall, our results demonstrate that reducing residential combustion emissions would have substantial benefits for human health through reductions in ambient PM2.5 concentrations.

The oxidation of biogenic volatile organic compounds (BVOCs) gives a range of products, from semi-volatile to extremely low-volatility compounds. To treat the interaction of these secondary organic vapours with the particle phase, global aerosol microphysics models generally use either a thermodynamic partitioning approach (assuming instant equilibrium between semi-volatile oxidation products and the particle phase) or a kinetic approach (accounting for the size dependence of condensation). We show that model treatment of the partitioning of biogenic organic vapours into the particle phase, and consequent distribution of material across the size distribution, controls the magnitude of the first aerosol indirect effect (AIE) due to biogenic secondary organic aerosol (SOA). With a kinetic partitioning approach, SOA is distributed according to the existing condensation sink, enhancing the growth of the smallest particles, i.e. those in the nucleation mode. This process tends to increase cloud droplet number concentrations in the presence of biogenic SOA. By contrast, an approach that distributes SOA according to pre-existing organic mass restricts the growth of the smallest particles, limiting the number that are able to form cloud droplets. With an organically mediated new particle formation mechanism, applying a mass-based rather than a kinetic approach to partitioning reduces our calculated global mean AIE due to biogenic SOA by 24 %. Our results suggest that the mechanisms driving organic partitioning need to be fully understood in order to accurately describe the climatic effects of SOA.

Emissions of biogenic volatile organic compounds (BVOCs) have changed in the past millennium due to changes in land use, temperature, and CO2 concentrations. Recent reconstructions of BVOC emissions have predicted that global isoprene emissions have decreased, while monoterpene and sesquiterpene emissions have increased; however, all three show regional variability due to competition between the various influencing factors. In this work, we use two modeled estimates of BVOC emissions from the years 1000 to 2000 to test the effect of anthropogenic changes to BVOC emissions on secondary organic aerosol (SOA) formation, global aerosol size distributions, and radiative effects using the GEOS-Chem-TOMAS (Goddard Earth Observing System; TwO-Moment Aerosol Sectional) global aerosol microphysics model. With anthropogenic emissions (e.g., SO2, NOx, primary aerosols) turned off and BVOC emissions changed from year 1000 to year 2000 values, decreases in the number concentration of particles of size Dp > 80 nm (N80) of > 25% in year 2000 relative to year 1000 were predicted in regions with extensive land-use changes since year 1000 which led to regional increases in the combined aerosol radiative effect (direct and indirect) of > 0.5 W m−2 in these regions. We test the sensitivity of our results to BVOC emissions inventory, SOA yields, and the presence of anthropogenic emissions; however, the qualitative response of the model to historic BVOC changes remains the same in all cases. Accounting for these uncertainties, we estimate millennial changes in BVOC emissions cause a global mean direct effect of between +0.022 and +0.163 W m−2 and the global mean cloud-albedo aerosol indirect effect of between −0.008 and −0.056 W m−2. This change in aerosols, and the associated radiative forcing, could be a largely overlooked and important anthropogenic aerosol effect on regional climates.

We use a global aerosol microphysics model in combination with an offline radiative transfer model to quantify the radiative effect of biogenic secondary organic aerosol (SOA) in the present-day atmosphere. Through its role in particle growth and ageing, the presence of biogenic SOA increases the global annual mean concentration of cloud condensation nuclei (CCN; at 0.2% supersaturation) by 3.6–21.1%, depending upon the yield of SOA production from biogenic volatile organic compounds (BVOCs), and the nature and treatment of concurrent primary carbonaceous emissions. This increase in CCN causes a rise in global annual mean cloud droplet number concentration (CDNC) of 1.9–5.2%, and a global mean first aerosol indirect effect (AIE) of between +0.01 W m−2 and −0.12 W m−2. The radiative impact of biogenic SOA is far greater when biogenic oxidation products also contribute to the very early stages of new particle formation; using two organically mediated mechanisms for new particle formation, we simulate global annual mean first AIEs of −0.22 W m−2 and −0.77 W m−2. The inclusion of biogenic SOA substantially improves the simulated seasonal cycle in the concentration of CCN-sized particles observed at three forested sites. The best correlation is found when the organically mediated nucleation mechanisms are applied, suggesting that the first AIE of biogenic SOA could be as large as −0.77 W m−2. The radiative impact of SOA is sensitive to the presence of anthropogenic emissions. Lower background aerosol concentrations simulated with anthropogenic emissions from 1750 give rise to a greater fractional CCN increase and a more substantial first AIE from biogenic SOA. Consequently, the anthropogenic indirect radiative forcing between 1750 and the present day is sensitive to assumptions about the amount and role of biogenic SOA. We also calculate an annual global mean direct radiative effect of between −0.08 W m−2 and −0.78 W m−2 in the present day, with uncertainty in the amount of SOA produced from the oxidation of BVOCs accounting for most of this range.

This study evaluates effects and applications of a new linear parameterisation for stratospheric methane and water vapour. The new scheme (CoMeCAT) is derived from a 3-D full-chemistry-transport model (CTM). It is suitable for any global model, and is shown here to produce realistic profiles in the TOMCAT/SLIMCAT 3-D CTM and the ECMWF (European Centre for Medium-Range Weather Forecasts) general circulation model (GCM). Results from the new scheme are in good agreement with the full-chemistry CTM CH4 field and with observations from the Halogen Occultation Experiment (HALOE). The scheme is also used to derive stratospheric water increments, which in the CTM produce vertical and latitudinal H2O variations in fair agreement with satellite observations. Stratospheric H2O distributions in the ECMWF GCM show realistic overall features, although concentrations are smaller than in the CTM run (up to 0.5 ppmv smaller above 10 hPa). The potential of the new CoMeCAT tracer for evaluating stratospheric transport is exploited to assess the impacts of nudging the free-running GCM to ERA-40 and ERA-Interim reanalyses. The nudged GCM shows similar transport patterns to the offline CTM forced by the corresponding reanalysis data. The new scheme also impacts radiation and temperature in the model. Compared to the default CH4 climatology and H2O used by the ECMWF radiation scheme, the main effect on ECMWF temperatures when considering both CH4 and H2O from CoMeCAT is a decrease of up to 1.0 K over the tropical mid/low stratosphere. The effect of using the CoMeCAT scheme for radiative forcing (RF) calculations is investigated using the offline Edwards–Slingo radiative transfer model. Compared to the default model option of a tropospheric global 3-D CH4 value, the CoMeCAT distribution produces an overall change in the annual mean net RF of up to −30 mW m−2.

The Mediterranean troposphere exhibits a marked and localised summertime ozone maximum, which has the potential to strongly impact regional air quality and radiative forcing. The Mediterranean region can be perturbed by long-range pollution import from Northern Europe, North America and Asia, in addition to local emissions, which may all contribute to regional ozone enhancements. We exploit ozone profile observations from the Tropospheric Emission Spectrometer (TES) and the Global Ozone Monitoring Experiment-2 (GOME-2) satellite instruments, and an offline 3-D global chemical transport model (TOMCAT) to investigate the geographical and vertical structure of the summertime tropospheric ozone maximum over the Mediterranean region. We show that both TES and GOME-2 are able to detect enhanced levels of ozone in the lower troposphere over the region during the summer. These observations, together with surface measurements, are used to evaluate the TOMCAT model's ability to capture the observed ozone enhancement. The model is used to quantify sensitivities of the ozone maximum to anthropogenic and natural volatile organic compound (VOC) emissions, anthropogenic NOx emissions, wildfire emissions and long-range import of ozone and precursors. Our results show a dominant sensitivity to natural VOC emissions in the Mediterranean basin over anthropogenic VOC emissions. However, local anthropogenic NOx emissions are result in the overall largest sensitivity in near-surface ozone. We also show that in the lower troposphere, global VOC emissions account for 40% of the ozone sensitivity to VOC emissions in the region, whereas, for NOx the ozone sensitivity to local sources is 9 times greater than that for global emissions at these altitudes. However, in the mid and upper troposphere ozone is most sensitive to non-local emission sources. In terms of radiative effects on regional climate, ozone contributions from non-local emission sources are more important, as these have a larger impact on ozone in the upper troposphere where its radiative effects are larger, with Asian monsoon outflow having the greatest impact. Our results allow improved understanding of the large-scale processes controlling air quality and climate in the region of the Mediterranean basin.

Contrails and especially their evolution into cirrus-like clouds are thought to have very important effects on local and global radiation budgets, though are generally not well represented in global climate models. Lack of contrail parameterisations is due to the limited availability of in situ contrail measurements which are difficult to obtain. Here we present a methodology for successful sampling and interpretation of contrail microphysical and radiative data using both in situ and remote sensing instrumentation on board the FAAM BAe146 UK research aircraft as part of the COntrails Spreading Into Cirrus (COSIC) study. Forecast models were utilised to determine flight regions suitable for contrail formation and sampling; regions that were both free of cloud but showed a high probability of occurrence of air mass being supersaturated with respect to ice. The FAAM research aircraft, fitted with cloud microphysics probes and remote sensing instruments, formed a distinctive spiral-shaped contrail in the predicted area by flying in an orbit over the same ground position as the wind advected the contrails to the east. Parts of these contrails were sampled during the completion of four orbits, with sampled contrail regions being between 7 and 30 min old. Lidar measurements were useful for in-flight determination of the location and spatial extent of the contrails, and also to report extinction values that agreed well with those calculated from the microphysical data. A shortwave spectrometer was also able to detect the contrails, though the signal was weak due to the dispersion and evaporation of the contrails. Post-flight the UK Met Office NAME III dispersion model was successfully used as a tool for modelling the dispersion of the persistent contrail; determining its location and age, and determining when there was interference from other measured aircraft contrails or when cirrus encroached on the area later in the flight. The persistent contrails were found to consist of small (~10 μm) plate-like crystals where growth of ice crystals to larger sizes (~100 μm) was typically detected when higher water vapour levels were present. Using the cloud microphysics data, extinction co-efficient values were calculated and found to be 0.01–1 km−1. The contrails formed during the flight (referred to as B587) were found to have a visible lifetime of ~40 min, and limited water vapour supply was thought to have suppressed ice crystal growth.

Observations and models have shown that continuously degassing volcanoes have a potentially large effect on the natural background aerosol loading and the radiative state of the atmosphere. We use a global aerosol microphysics model to quantify the impact of these volcanic emissions on the cloud albedo radiative forcing under pre-industrial (PI) and present-day (PD) conditions. We find that volcanic degassing increases global annual mean cloud droplet number concentrations by 40% under PI conditions, but by only 10% under PD conditions. Consequently, volcanic degassing causes a global annual mean cloud albedo effect of −1.06 W m−2 in the PI era but only −0.56 W m−2 in the PD era. This non-equal effect is explained partly by the lower background aerosol concentrations in the PI era, but also because more aerosol particles are produced per unit of volcanic sulphur emission in the PI atmosphere. The higher sensitivity of the PI atmosphere to volcanic emissions has an important consequence for the anthropogenic cloud radiative forcing because the large uncertainty in volcanic emissions translates into an uncertainty in the PI baseline cloud radiative state. Assuming a −50/+100% uncertainty range in the volcanic sulphur flux, we estimate the annual mean anthropogenic cloud albedo forcing to lie between −1.16 W m−2 and −0.86 W m−2. Therefore, the volcanically induced uncertainty in the PI baseline cloud radiative state substantially adds to the already large uncertainty in the magnitude of the indirect radiative forcing of climate.

The budget of atmospheric secondary organic aerosol (SOA) is very uncertain, with recent estimates suggesting a global source of between 12 and 1820 Tg (SOA) a−1. We used a dataset of aerosol mass spectrometer (AMS) observations from 34 different surface locations to evaluate the GLOMAP global chemical transport model. The standard model simulation (which included SOA from monoterpenes only) underpredicted organic aerosol (OA) observed by the AMS and had little skill reproducing the variability in the dataset. We simulated SOA formation from biogenic (monoterpenes and isoprene), lumped anthropogenic and lumped biomass burning volatile organic compounds (VOCs) and varied the SOA yield from each precursor source to produce the best overall match between model and observations. We assumed that SOA is essentially non-volatile and condenses irreversibly onto existing aerosol. Our best estimate of the SOA source is 140 Tg (SOA) a−1 but with a large uncertainty range which we estimate to be 50–380 Tg (SOA) a−1. We found the minimum in normalised mean error (NME) between model and the AMS dataset when we assumed a large SOA source (100 Tg (SOA) a−1) from sources that spatially matched anthropogenic pollution (which we term antropogenically controlled SOA). We used organic carbon observations compiled by Bahadur et al. (2009) to evaluate our estimated SOA sources. We found that the model with a large anthropogenic SOA source was the most consistent with these observations, however improvement over the model with a large biogenic SOA source (250 Tg (SOA) a−1) was small. We used a dataset of 14C observations from rural locations to evaluate our estimated SOA sources. We estimated a maximum of 10 Tg (SOA) a−1 (10 %) of the anthropogenically controlled SOA source could be from fossil (urban/industrial) sources. We suggest that an additional anthropogenic source is most likely due to an anthropogenic pollution enhancement of SOA formation from biogenic VOCs. Such an anthropogenically controlled SOA source would result in substantial climate forcing. We estimated a global mean aerosol direct effect of −0.26 ± 0.15 Wm−2 and indirect (cloud albedo) effect of −0.6+0.24−0.14 Wm−2 from anthropogenically controlled SOA. The biogenic and biomass SOA sources are not well constrained with this analysis due to the limited number of OA observations in regions and periods strongly impacted by these sources. To further improve the constraints by this method, additional OA observations are needed in the tropics and the Southern Hemisphere.

Black carbon in carbonaceous combustion aerosol warms the climate by absorbing solar radiation, meaning reductions in black carbon emissions are often perceived as an attractive global warming mitigation option. However, carbonaceous combustion aerosol can also act as cloud condensation nuclei (CCN) so they also cool the climate by increasing cloud albedo. The net radiative effect of carbonaceous combustion aerosol is uncertain because their contribution to CCN has not been evaluated on the global scale. By combining extensive observations of CCN concentrations with the GLOMAP global aerosol model, we find that the model is biased low (normalised mean bias = −77 %) unless carbonaceous combustion aerosol act as CCN. We show that carbonaceous combustion aerosol accounts for more than half (52–64 %) of global CCN with the range due to uncertainty in the emitted size distribution of carbonaceous combustion particles. The model predicts that wildfire and pollution (fossil fuel and biofuel) carbonaceous combustion aerosol causes a global mean cloud albedo aerosol indirect effect of −0.34 W m−2, with stronger cooling if we assume smaller particle emission size. We calculate that carbonaceous combustion aerosol from pollution sources cause a global mean aerosol indirect effect of −0.23 W m−2. The small size of carbonaceous combustion particles from fossil fuel sources means that whilst pollution sources account for only one-third of the emitted mass they cause two-thirds of the cloud albedo aerosol indirect effect that is due to carbonaceous combustion aerosol. This cooling effect must be accounted for, along with other cloud effects not studied here, to ensure that black carbon emissions controls that reduce the high number concentrations of fossil fuel particles have the desired net effect on climate.

The release of vast quantities of methane into the atmosphere as a result of clathrate destabilization is a potential mechanism for rapid amplification of global warming. Previous studies have calculated the enhanced warming based mainly on the radiative effect of the methane itself, with smaller contributions from the associated carbon dioxide or ozone increases. Here, we study the effect of strongly elevated methane (CH4) levels on oxidant and aerosol particle concentrations using a combination of chemistry-transport and general circulation models. A 10-fold increase in methane concentrations is predicted to significantly decrease hydroxyl radical (OH) concentrations, while moderately increasing ozone (O3). These changes lead to a 70 % increase in the atmospheric lifetime of methane, and an 18 % decrease in global mean cloud droplet number concentrations (CDNC). The CDNC change causes a radiative forcing that is comparable in magnitude to the longwave radiative forcing ("enhanced greenhouse effect") of the added methane. Together, the indirect CH4-O3 and CH4-OH-aerosol forcings could more than double the warming effect of large methane increases. Our findings may help explain the anomalously large temperature changes associated with historic methane releases.

Chemical escape rooms (ChEsRms) are educational games in which students use their brain, chemical knowledge, intuition, and a bit of luck to solve a mystery. At the Weizmann Institute, we have developed ChEsRms that are implemented by teachers in their classes. Since the COVID-19 pandemic stopped all the educational activities that took place in physical space, we decided to design a virtual ChEsRm (VChEsRm) that is fully conducted in digital space. We describe the design principles that characterize the VChEsRm and present the students' and teachers' perceptions of the VChEsRm and how it differs from the ChEsRm. We describe "The Masked Scientist", a VChEsRm in which students must identify a scientist using their knowledge of basic topics in the chemistry syllabus: the model of the atom, radioactivity, and the periodic table. This VChEsRm has added values, a connection to history, human rights, and sustainability, as well as interesting and surprising chemical facts related to everyday life. Since it is conducted in virtual space, it could also include experiments, procedures, and materials that are dangerous and therefore forbidden in a physical ChEsRm or that could even change the course of history. Importantly, this 90 min activity includes the VChEsRm (9 puzzles) and a 45 min follow-up session that deals with the ideas behind the puzzles. It was translated from Hebrew to Arabic and English; therefore, high school and general chemistry teachers around the world can easily use the VChEsRm in their class after reading this paper by clicking on the link.