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A new experimental system is described for studying the pyrolysis of the refractory organic constituents in cosmic dust during atmospheric entry. The pyrolysis kinetics of meteoritic fragments (CM2 and CV3 carbonaceous chondrites, radius = 36–100 μm) were measured by mass spectrometric detection of CO2 and SO2 at temperatures between 625 and 1300 K, with most carbon being lost between 700 and 800 K. The complex time-resolved kinetic behavior is consistent with two organic components—one significantly more refractory than the other, which probably correspond to the insoluble and soluble organic fractions, respectively. The measured temperature-dependent pyrolysis rates were then incorporated into the Leeds Chemical Ablation Model, which demonstrates that organic pyrolysis should be detectable using a high performance/large aperture radar. Atomic force microscopy was used to show that although the residual meteoritic particles became more brittle after organic pyrolysis, they also became slightly harder, withstanding stresses that are at least three orders of magnitude higher than would be encountered during atmospheric entry. This suggests that most cosmic dust particles (radius

Accurately quantifying volcanic impacts on climate is a key requirement for robust attribution of anthropogenic climate change. Here we use the Unified Model – United Kingdom Chemistry and Aerosol (UM-UKCA) composition–climate model to simulate the global dispersion of the volcanic aerosol clouds from the three largest eruptions of the 20th century: 1963 Mt Agung, 1982 El Chichón, and 1991 Mt Pinatubo. The model has interactive stratospheric chemistry and aerosol microphysics, with coupled aerosol–radiation interactions for realistic composition–dynamics feedbacks. Our simulations align with the design of the Interactive Stratospheric Aerosol Model Intercomparison (ISA-MIP) “Historical Eruption SO2 Emissions Assessment”. For each eruption, we perform three-member ensemble model experiments for upper, mid-point, and lower estimates of SO2 emission, each re-initialised from a control run to approximately match the observed transition in the phase of the quasi-biennial oscillation (QBO) in the 6 months after the eruptions. With this experimental design, we assess how each eruption's emitted SO2 translates into a tropical reservoir of volcanic aerosol and analyse the subsequent dispersion to mid-latitudes. We compare the simulations to the volcanic forcing datasets (e.g. Space-based Stratospheric Aerosol Climatology (GloSSAC); Sato et al., 1993, and Ammann et al., 2003) that are used in historical integrations for the two most recent Coupled Model Intercomparison Project (CMIP) assessments. For Pinatubo and El Chichón, we assess the vertical extent of the simulated volcanic clouds by comparing modelled extinction to the Stratospheric Aerosol and Gas Experiment (SAGE-II) v7.0 satellite measurements and to 1964–1965 Northern Hemisphere ground-based lidar measurements for Agung. As an independent test for the simulated volcanic forcing after Pinatubo, we also compare simulated shortwave (SW) and longwave (LW) top-of-the-atmosphere radiative forcings to the flux anomalies measured by the Earth Radiation Budget Experiment (ERBE) satellite instrument. For the Pinatubo simulations, an injection of 10 to 14 Tg SO2 gives the best match to the High Resolution Infrared Sounder (HIRS) satellite-derived global stratospheric sulfur burden, with good agreement also with SAGE-II mid-visible and near-infra-red extinction measurements. This 10–14 Tg range of emission also generates a heating of the tropical stratosphere that is consistent with the temperature anomaly present in the ERA-Interim reanalysis. For El Chichón, the simulations with 5 and 7 Tg SO2 emission give best agreement with the observations. However, these simulations predict a much deeper volcanic cloud than represented in the GloSSAC dataset, which is largely based on an interpolation between Stratospheric Aerosol Measurements (SAM-II) satellite and aircraft measurements. In contrast, these simulations show much better agreement during the SAGE-II period after October 1984. For 1963 Agung, the 9 Tg simulation compares best to the forcing datasets with the model capturing the lidar-observed signature of the altitude of peak extinction descending from 20 km in 1964 to 16 km in 1965. Overall, our results indicate that the downward adjustment to SO2 emission found to be required by several interactive modelling studies when simulating Pinatubo is also needed when simulating the Agung and El Chichón aerosol clouds. This strengthens the hypothesis that interactive stratospheric aerosol models may be missing an important removal or re-distribution process (e.g. effects of co-emitted ash) which changes how the tropical reservoir of volcanic aerosol evolves in the initial months after an eruption. Our model comparisons also identify potentially important inhomogeneities in the CMIP6 dataset for all three eruption periods that are hard to reconcile with variations predicted in the interactive stratospheric aerosol simulations. We also highlight large differences between the CMIP5 and CMIP6 volcanic aerosol datasets for the Agung and El Chichón periods. Future research should aim to reduce this uncertainty by reconciling the datasets with additional stratospheric aerosol observations.

The accumulation rate of meteoric smoke particles (MSPs) in ice cores—determined from the trace elements Ir and Pt, and superparamagnetic Fe particles—is significantly higher than expected from the measured vertical fluxes of Na and Fe atoms in the upper mesosphere and the surface deposition of cosmic spherules. The Whole Atmosphere Community Climate Model with the Community Aerosol and Radiation Model for Atmospheres has been used to simulate MSP production, transport, and deposition, using a global MSP input of 7.9 t d⁻¹ based on these other measurements. The modeled MSP deposition rates are smaller than the measurements by factors of ~32 in Greenland and ~12 in Antarctica, even after reanalysis of the Ir/Pt ice core data with inclusion of a volcanic source. Variations of the model deposition scheme and use of the United Kingdom Chemistry and Aerosols model do not improve the agreement. Direct removal of MSP‐nucleated polar stratospheric cloud particles to the surface gives much better agreement, but would result in an unfeasibly high rate of nitrate deposition. The unablated fraction of cosmic dust (~35 t d⁻¹) would provide sufficient Ir and Pt to account for the Antarctic measurements, but the relatively small flux of these large (>3 μm) particles would lead to greater variability in the ice core measurements than is observed, although this would be partly offset if significant fragmentation of cosmic dust particles occurred during atmospheric entry. Future directions to resolve these discrepancies between models and measurements are also discussed.

Novel methodologies to quantify model uncertainty are combined with an extensive new database of in-situ aerosol microphysical and chemical measurements to reduce uncertainty in aerosol effects on climate. The largest uncertainty in the historical radiative forcing of climate is caused by changes in aerosol particles due to anthropogenic activity. Sophisticated aerosol microphysics processes have been included in many climate models in an effort to reduce the uncertainty. However, the models are very challenging to evaluate and constrain because they require extensive in-situ measurements of the particle size distribution, number concentration and chemical composition that are not available from global satellite observations. The Global Aerosol Synthesis and Science Project (GASSP) aims to improve the robustness of global aerosol models by combining new methodologies for quantifying model uncertainty, an extensive global dataset of aerosol in-situ microphysical and chemical measurements, and new ways to assess the uncertainty associated with comparing sparse point measurements with low resolution models. GASSP has assembled over 45,000 hours of measurements from ships and aircraft as well as data from over 350 ground stations. The measurements have been harmonized into a standardized format that is easily used by modellers and non-specialist users. Available measurements are extensive, but they biased to polluted regions of the northern hemisphere, leaving large pristine regions and many continental areas poorly sampled. The aerosol radiative forcing uncertainty can be reduced using a rigorous model-data synthesis approach. Nevertheless, our research highlights significant remaining challenges because of the difficulty of constraining many interwoven model uncertainties simultaneously. Although the physical realism of global aerosol models still needs to be improved, the uncertainty in aerosol radiative forcing will be reduced most effectively by systematically and rigorously constraining the models using extensive syntheses of measurements.

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.

Aerosols are short lived so their geographical distribution and impact on climate depends on where they are emitted. Previous model studies have shown that the mass of sulfate aerosol produced per unit sulfur emission (the sulfate burden potential) and the associated direct radiative forcing vary regionally because of differences in meteorology and photochemistry. Using a global model of aerosol microphysics, we show that the total number of aerosol particles produced per unit sulfur emission (the aerosol number potential) has a different regional variation to that of sulfate mass. The aerosol number potential of N. American and Asian emissions is calculated to be a factor of 3 to 4 times greater than that of European emissions, even though Europe has a higher sulfate burden potential. Pollution from North America and Asia tends to reach higher altitudes than European pollution so forms more new particles through nucleation. These regional differences in particle production mean that sulfur emissions from N. America and E. Asia produce cloud condensation nuclei up to 70% more efficiently than Europe. Taking account of the higher sulfate burden potential of Europe in these simulations shows that E. Asian sulfate produces CCN twice as effectively as European sulfate. The impact of regional sulfur emissions on particle concentrations is also much more widely spread than the impact on sulfate mass, due to efficient particle production in the free troposphere during long range transport. These results imply that regional sulfur emissions will have different climate forcing potentials through changes in cloud drop number.

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 < 2.5 μm) and on the global radiation budget due to changes in aerosol and tropospheric ozone. We estimate that present-day non-CO2 aviation emissions with a typical FSC of 600 ppm result in 3597 (95 % CI: 1307–5888) annual 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 624 (95 % CI: 227–1021) mortalities a−1 and increase REcomb by +7.0 mW m−2. We explore the impact of varying aviation FSC between 0–6000 ppm. Increasing FSC increases annual mortality, while enhancing climate cooling through increasing the aerosol cloud albedo effect (aCAE). 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 aCAE. Aviation emissions injected at the surface are 5 times less effective at forming cloud condensation nuclei, reducing the aviation-induced aCAE by a factor of 10. Applying high FSCs at aviation cruise altitudes combined with ULSJ fuel at lower altitudes result in reduced aviation-induced mortality and increased negative RE compared to the baseline aviation scenario.

Following the eruption of Mt. Pinatubo, satellite and in-situ measurements showed a large enhancement in stratospheric aerosol in both hemispheres, but significant mid-latitude column O3 depletion was observed only in the north. We use a three-dimensional chemical transport model to determine the mechanisms behind this hemispheric asymmetry. The model, forced by European Centre for Medium-Range Weather Forecasts ERA-Interim reanalyses and updated aerosol surface area density, successfully simulates observed large column NO2 decreases and the different extents of ozone depletion in the two hemispheres. The chemical ozone loss is similar in the northern (NH) and southern hemispheres (SH), but the contrasting role of dynamics increases the depletion in the NH and decreases it in the SH. The relevant SH dynamics are not captured as well by earlier ERA-40 reanalyses. Overall the smaller SH column O3 depletion can be attributed to dynamical variability and smaller SH background lower stratosphere O3 concentrations.

Aerosols and their effect on the radiative properties of clouds are one of the largest sources of uncertainty in calculations of the Earth's energy budget. Here the sensitivity of aerosol-cloud albedo effect forcing to 31 aerosol parameters is quantified. Sensitivities are compared over three periods; 1850-2008, 1978-2008, and 1998-2008. Despite declining global anthropogenic SO2 emissions during 1978-2008, a cancelation of regional positive and negative forcings leads to a near-zero global mean cloud albedo effect forcing. In contrast to existing negative estimates, our results suggest that the aerosol-cloud albedo effect was likely positive (0.006 to 0.028Wm-2) in the recent decade, making it harder to explain the temperature hiatus as a forced response. Proportional contributions to forcing variance from aerosol processes and natural and anthropogenic emissions are found to be period dependent. To better constrain forcing estimates, the processes that dominate uncertainty on the timescale of interest must be better understood. Key Points Forcing sensitivity to aerosol parameters is strongly period dependentUnderstanding near-future climate is limited if a single period is consideredIn recent decades, parametric uncertainty is smaller than model diversity

A global model of aerosol microphysics is used to simulate a large East Asian dust storm during the ACE-Asia experiment. We use the model together with size resolved measurements of aerosol number concentration and composition to examine how dust modified the production of sulfate aerosol and the particle size distribution in East Asian outflow. Simulated size distributions and mass concentrations of dust, sub- and super-micron sulfate agree well with observations from the C-130 aircraft. Modeled mass concentrations of fine sulfate (DpDp>1.0 μm) by more than an order of magnitude, but total sulfate concentrations increase by less than 2% because decreases in fine sulfate have a compensating effect. Our analysis shows that the sulfate associated with dust can be explained largely by the uptake of H2SO4 rather than reaction of SO2 on the dust surface, which we assume is suppressed once the particles are coated in sulfate. We suggest that many previous model investigations significantly overestimated SO2 oxidation on East Asian dust, possibly due to the neglect of surface saturation effects. We extend previous model experiments by examining how dust modified existing particle concentrations in Asian outflow. Total particle concentrations (condensation nuclei, CN) modeled in the dust-pollution plume are reduced by up to 20%, but we predict that dust led to less than 10% depletion in particles large enough to act as cloud condensation nuclei (CCN). Our analysis suggests that E. Asian dust storms have only a minor impact on sulfate particles present at climate-relevant sizes.

International audience; Denitrification of the Arctic winter stratosphere has been calculated using a 3-D microphysical model for the winters 1994/95, 1995/96, 1996/97 and 1999/2000. Denitrification is assumed to occur through the sedimentation of low number concentrations of large nitric acid trihydrate (NAT) particles (as inferred by e.g. Fahey et al., 2001). We examine whether the meteorological conditions that allowed particles to grow to the very large sizes observed in 1999/2000 also occurred in the other cold winters. The results show that winter 1999/2000 had conditions that were optimum for denitrification by large NAT particles, which are a deep concentric NAT area and vortex. Under these conditions, NAT particles can circulate in the NAT-supersaturated air for several days, reaching several micrometres in radius and leading to a high downward flux of nitric acid. The other winters had shorter periods with optimum conditions for denitrification. However, we find that NAT particles could have grown to large sizes in all of these winters and could have caused significant denitrification. We define the quantity "closed-flow area'' (the fraction of the NAT area in which air parcel trajectories can form closed loops) and show that it is a very useful indicator of possible denitrification. We find that even with a constant NAT nucleation rate throughout the NAT area, the average NAT number concentration and size can vary by up to a factor of 10 in response to this meteorological quantity. These changes in particle properties account for a high degree of variability in denitrification between the different winters. This large meteorologically induced variability in denitrification rate needs to be compared with that which could arise from a variable nucleation rate of NAT particles, which remains an uncertain quantity in models. Sensitivity studies show that although denitrification was likely approaching asymptotic minimum values throughout much of the 1999/2000 vortex, decreases in the volume-averaged nucleation rate would have substantially reduced the denitrification.

Funder: U.K. China Research and Innovation Partnership Fund, Funder: National Centre for Atmospheric Science (NCAS); Id: http://dx.doi.org/10.13039/501100000662, Reconstructions of volcanic aerosol radiative forcing are required to understand past climate variability. Currently, reconstructions of pre‐20th century volcanic forcing are derived from sulfate concentrations measured in polar ice cores, mainly using a relationship between the average ice‐sheet sulfate deposition and stratospheric sulfate aerosol burden based on a single explosive eruption—the 1991 eruption of Mt. Pinatubo. Here we estimate volcanic radiative forcings and associated uncertainty ranges from ice‐core sulfate records of eight of the largest bipolar deposition signals in the last 2,500 years using statistical emulation of a perturbed parameter ensemble of aerosol‐climate model simulations of explosive eruptions. Extensive sampling of different combinations of eruption source parameters using the emulators reveals that a very wide range of eruptions in different seasons with different sulfur dioxide emissions, eruption latitudes, and emission altitudes produce ice‐sheet sulfate deposition consistent with ice‐core records. Consequently, we find a large range in the volcanic forcing that can be directly attributed to the unknown eruption source parameters. We estimate that the uncertainty in volcanic forcing caused by many plausible eruption realizations leads to uncertainties in the global mean surface cooling of around 1°C for the largest unidentified historical eruptions. Our emulators are available online (https://cemac.github.io/volcanic-forcing-deposition) where eruption realizations for given ice‐sheet sulfate depositions can be explored.