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​​​​​​​The 21 June 2019 Raikoke eruption (48° N, 153° E) generated one of the largest amounts of sulfur emission to the stratosphere since the 1991 Mt. Pinatubo eruption. Satellite measurements indicate a consensus best estimate of 1.5 Tg for the sulfur dioxide (SO 2) injected at an altitude of around 14–15 km. The peak Northern Hemisphere (NH) mean 525 nm stratospheric aerosol optical depth (SAOD) increased to 0.025, a factor of 3 higher than background levels. The Volcano Response (VolRes) initiative provided a platform for the community to share information about this eruption which significantly enhanced coordination efforts in the days after the eruption. A multi-platform satellite observation subgroup formed to prepare an initial report to present eruption parameters including SO 2 emissions and their vertical distribution for the modeling community. It allowed us to make the first estimate of what would be the peak in SAOD 1 week after the eruption using a simple volcanic aerosol model. In this retrospective analysis, we show that revised volcanic SO 2 injection profiles yield a higher peak injection of the SO 2 mass. This highlights difficulties in accurately representing the vertical distribution for moderate SO 2 explosive eruptions in the lowermost stratosphere due to limited vertical sensitivity of the current satellite sensors (± 2 km accuracy) and low horizontal resolution of lidar observations. We also show that the SO 2 lifetime initially assumed in the simple aerosol model was overestimated by 66 %, pointing to challenges for simple models to capture how the life cycle of volcanic gases and aerosols depends on the SO 2 injection magnitude, latitude, and height. Using a revised injection profile, modeling results indicate a peak NH monthly mean SAOD at 525 nm of 0.024, in excellent agreement with observations, associated with a global monthly mean radiative forcing of - 0.17 W m -2 resulting in an annual global mean surface temperature anomaly of - 0.028 K. Given the relatively small magnitude of the forcing, it is unlikely that the surface response can be dissociated from surface temperature variability. [ABSTRACT FROM AUTHOR]

A growing number of general circulation models are adapting interactive sulfur and aerosol schemes to improve the representation of relevant physical and chemical processes and associated feedbacks. They are motivated by investigations of climate response to major volcanic eruptions and potential solar geoengineering scenarios. However, uncertainties in these schemes are not well constrained. Stratospheric sulfate is modulated by emissions of sulfur-containing species of anthropogenic and natural origin, including volcanic activity. While the effects of volcanic eruptions have been studied in the framework of global model intercomparisons, the background conditions of the sulfur cycle have not been addressed in such a way. Here, we fill this gap by analyzing the distribution of the main sulfur species in nine global atmospheric aerosol models for a volcanically quiescent period. We use observational data to evaluate model results. Overall, models agree that the three dominant sulfur species in terms of burdens (sulfate aerosol, OCS, and SO 2) make up about 98 % stratospheric sulfur and 95 % tropospheric sulfur. However, models vary considerably in the partitioning between these species. Models agree that anthropogenic emission of SO 2 strongly affects the sulfate aerosol burden in the northern hemispheric troposphere, while its importance is very uncertain in other regions, where emissions are much lower. Sulfate aerosol is the main deposited species in all models, but the values deviate by a factor of 2. Additionally, the partitioning between wet and dry deposition fluxes is highly model dependent. Inter-model variability in the sulfur species is low in the tropics and increases towards the poles. Differences are largest in the dynamically active northern hemispheric extratropical region and could be attributed to the representation of the stratospheric circulation. The differences in the atmospheric sulfur budget among the models arise from the representation of both chemical and dynamical processes, whose interplay complicates the bias attribution. Several problematic points identified for individual models are related to the specifics of the chemistry schemes, model resolution, and representation of cross-tropopause transport in the extratropics. Further model intercomparison research is needed with a focus on the clarification of the reasons for biases, given the importance of this topic for the stratospheric aerosol injection studies. [ABSTRACT FROM AUTHOR]

Sulfate aerosol in the stratosphere is an important climate driver, causing solar dimming in the years after major volcanic eruptions. Hence, a growing number of general circulation models are adapting interactive sulfur and aerosol schemes to improve the representation of relevant chemical processes and associated feedbacks. However, uncertainties of these schemes are not well constrained. Stratospheric sulfate is modulated by natural emissions of sulfur-containing species, including volcanic eruptive, and anthropogenic emissions. Model intercomparisons have examined the effects of volcanic eruptions, whereas the background conditions of the sulfur cycle have not been addressed in a global model intercomparison project. Assessing background conditions in global models allows us to identify model discrepancies as they are masked by large perturbations such as volcanic eruptions, yet may still matter in the aftermath of such a disturbance. Here, we analyze the atmospheric burden, seasonal cycle, and vertical and meridional distribution of the main sulfur species among nine global atmospheric aerosol models that are widely used in the stratospheric aerosol research community. We use observational and reanalysis data to evaluate model results. Overall, models agree that the three dominant sulfur species in terms of burdens (sulfate aerosol, OCS, and SO2) make up about 98 % of stratospheric sulfur and 95 % of tropospheric sulfur. However, models vary considerably in the partitioning between these species. Models agree that anthropogenic emission of SO2 strongly affects the sulfate aerosol burden in the Northern Hemispheric troposphere, while its importance is very uncertain in other regions. The total deposition of sulfur varies among models, deviating by a factor of two, but models agree that sulfate aerosol is the main form in which sulfur is deposited. Additionally, the partitioning between wet and dry deposition fluxes is highly model dependent. We investigate the areas of greatest variability in the sulfur species burdens and find that inter-model variability is low in the tropics and increases towards the poles. Seasonality in the southern hemisphere is depicted very similar among models. Differences are largest in the dynamically active northern hemispheric extratropical region, hence some of the differences could be attributed to the differences in the representation of the stratospheric circulation among underlying general circulation models. This study highlights that the differences in the atmospheric sulfur budget among the models arise from the representation of both chemical and dynamical processes, whose interplay complicates the bias attribution. Several problematic points identified for individual models are related to the specifics of the chemistry schemes, model resolution, and representation of cross-tropopause transport in the extratropics. Further model intercomparison research is needed focusing on the clarification of the reasons for biases, given also the importance of this topic for the stratospheric aerosol injection studies. [ABSTRACT FROM AUTHOR]

The 21st June 2019 Raikoke eruption (48° N,153° E) generated one of the largest amounts of sulfur emission to the stratosphere since the 1991 Mt Pinatubo eruption. Satellite measurements indicate a consensus best estimate of 1.5 Tg for the sulfur dioxide (SO2) injected at an altitude of around 14–15 km. The peak northern hemisphere mean 525 nm Stratospheric Aerosol Optical Depth (SAOD) increased to 0.025, a factor of three higher than background levels. The Volcano Response (VolRes) initiative provided a platform for the community to share information about this eruption, which significantly enhanced coordination efforts in the days after the eruption. A multi-platform satellite observation sub-group formed to prepare an initial report to present eruption parameters including SO2 emissions and their vertical distribution for the modelling community. It allowed to make the first estimate of what would be the peak in SAOD one week after the eruption using a simple volcanic aerosol model. In this retrospective analysis, we show that revised volcanic SO2 injection profiles yield a higher peak injection of the SO2 mass. This highlights difficulties in accurately representing the vertical distribution for moderate SO2 explosive eruptions in the lowermost stratosphere due to limited vertical sensitivity of current satellite sensors (+/- 2 km accuracy) and low horizontal resolution of lidar observations. We also show that the SO2 lifetime initially assumed in the simple aerosol model was overestimated by 66 %, pointing to challenges for simple models to capture how the life cycle of volcanic gases and aerosols depends on the SO2 injection magnitude, latitude and height. Using revised injection profile, modelling results indicate a peak northern hemisphere monthly mean SAOD at 525 nm of 0.024, in excellent agreement with observations, associated with a global monthly mean radiative forcing of -0.17 W/m2 resulting in an annual global mean surface temperature anomalies of -0.028 K. Given the relatively small magnitude of the forcing, it is unlikely that the surface response can be dissociated from surface temperature variability. [ABSTRACT FROM AUTHOR]

The crystal formation of nitric acid trihydrate (NAT) in the absence of water ice is important for a subset of polar stratospheric clouds (PSCs) and thereby ozone depletion. It has been suggested that either fragmented meteoroids or meteoric smoke particles (MSPs), or possibly both, are important as heterogeneous nuclei of these crystals. Previous work has focused on the nucleating ability of meteoric material in nitric acid in the absence of sulfuric acid. However, it is known that when immersed in stratospheric sulfuric acid droplets, metal-containing meteoric material particles partially dissolve and components can reprecipitate as silica and alumina that have different morphologies to the original meteoric material. Hence, in this study, we experimentally and theoretically explore the relative role that sulfuric acid-processed MSPs and meteoric fragments may play in NAT nucleation in PSCs. We compared meteoric fragments that had recently been prepared (by milling a meteorite sample) to a sample annealed under conditions designed to simulate heating during entry into the Earth's atmosphere. Whilst the addition of sulfuric acid decreased the nucleating ability of the recently milled meteoric material relative to nucleation in binary nitric acid-water solutions (at similar NAT saturation ratio), the annealed meteoric fragments nucleated NAT with a similar effectiveness in both solutions. However, combining our results with measured fluxes of meteoric material to the Earth, sedimentation modelling and recent experiments on fragmentation of incoming meteoroids suggests that it is unlikely for there to be sufficient fragments to contribute to the nucleation of crystalline NAT particles. We then considered silica formed from sulfuric acid-processed MSPs. Our previous work showed that nanoparticulate silica (radius ∼6 nm) is a relatively poor promoter of nucleation compared with micron-scaled silica particles, which were more effective. Both materials have similar chemical and structural (crystallographically amorphous) properties, indicating that size is critical. Here, we account for surface curvature of primary grains using the Classical Nucleation Theory (CNT) to explore this size dependence. This model is able to explain the discrepancy in nucleation effectiveness of fumed silica and fused quartz by treating their nucleating activity (contact angle) as equal but with differing particle size (or surface curvature), assuming interfacial energies that are physically reasonable. Here, we use this CNT model to present evidence that nucleation of NAT on acid-processed MSPs, where the primary grain size is tens of nanometres, is also effective enough to contribute to NAT crystals in early season PSCs where there is an absence of ice. This study demonstrates that the modelling of crystal nucleation in PSCs and resulting ozone depletion relies on an accurate understanding of the transport and chemical processing of MSPs. This will affect estimated sensitivity of stratospheric chemistry to rare events such as large volcanic eruptions and long-term forecasting of ozone recovery in a changing climate. [ABSTRACT FROM AUTHOR]

A previous model intercomparison of the Tambora aerosol cloud has highlighted substantial differences among simulated volcanic aerosol properties in the pre-industrial stratosphere and has led to questions about the applicability of global aerosol models for large-magnitude explosive eruptions prior to the observational period. Here, we compare the evolution of the stratospheric aerosol cloud following the well-observed June 1991 Mt. Pinatubo eruption simulated with six interactive stratospheric aerosol microphysics models to a range of observational data sets. Our primary focus is on the uncertainties regarding initial SO 2 emission following the Pinatubo eruption, as prescribed in the Historical Eruptions SO 2 Emission Assessment experiments (HErSEA), in the framework of the Interactive Stratospheric Aerosol Model Intercomparison Project (ISA-MIP). Six global models with interactive aerosol microphysics took part in this study: ECHAM6-SALSA, EMAC, ECHAM5-HAM, SOCOL-AERv2, ULAQ-CCM, and UM-UKCA. Model simulations are performed by varying the SO 2 injection amount (ranging between 5 and 10 Tg S) and the altitude of injection (between 18–25 km). The comparisons show that all models consistently demonstrate faster reduction from the peak in sulfate mass burden in the tropical stratosphere. Most models also show a stronger transport towards the extratropics in the Northern Hemisphere, at the expense of the observed tropical confinement, suggesting a much weaker subtropical barrier in all the models, which results in a shorter e-folding time compared to the observations. Furthermore, simulations in which more than 5 Tg S in the form of SO 2 is injected show an initial overestimation of the sulfate burden in the tropics and, in some models, in the Northern Hemisphere and a large surface area density a few months after the eruption compared to the values measured in the tropics and the in situ measurements over Laramie. This draws attention to the importance of including processes such as the ash injection for the removal of the initial SO 2 and aerosol lofting through local heating. [ABSTRACT FROM AUTHOR]

We report the recovery and re-calibration of an extensive dataset of vertical profile measurements of the 1963/64 stratospheric aerosol layer measured from a two-site searchlight measurement facility at White Sands missile base and Sacramento Peak observatory, in New Mexico, US. The recovered dataset comprises 105 profiles of 550nm aerosol extinction (βp(z)) and is part of a longer program of measurements with the US Air Force Cambridge Research Laboratories (AFCRL) searchlight facility that began in February 1963. The recovered series of βp(z) profiles span the 13-month period December 1963 to December 1964 and provide a unique record of the altitude and vertical extent of the Northern Hemisphere dispersed portion of the aerosol cloud from the March 1963 Agung volcanic eruption. The data recovery methodology involved first re-digitizing the 105 original βp(z) profiles (βp(z)) from individual Figures within an AFCRL research report (Elterman, 1966a). The re-calibration involves inverting the original equation used to compute βp(z) in Elterman (1966a; 1966b) to retrieve a normalized detector response (Er(z) Er(35)) profile for each of the 105 re-digitized βp 0(z) profiles. An iterative procedure was then used to compute the re-calibration βp(z) profiles (βp Ra(z)), with the molecular extinction profile calculated with the corresponding daily molecular extinction profile calculated from local soundings, rather than the US Standard Atmosphere 1962 in the original dataset. Two-way molecular and aerosol transmittance corrections are applied using the MODTRAN (MODerate resolution atmospheric TRANsmission) code in transmission mode, applying a best-estimate aerosol phase function calculated from measurements, applied for the entire 2.76 to 35.2 km column. For the tropospheric aerosol transmittance, the AERONET aerosol phase function from White Sands High Energy Laser Systems Test Facility (HELSTF) was applied (2.76 to 10.7 km), a separate stratospheric phase function applied between 11.2 and 35.2 km, calculated from a set of particle size distributions measured by the U-2 high-altitude aircraft over a US region in the vicinity of White Sands in early 1964. Errors were estimated taking as a reference the errors determined in the computation of βp 0(z). Using available tabulated data from the original procedure the errors in the re-digitalization of βp 0(z) and in the retrieval of the Er(z) Er(35) procedures were calculated and later added to the original estimates. Both the βp R(z) and the stratospheric aerosol optical depth magnitudes showed higher magnitudes than βp 0(z) and the original stratospheric aerosol optical depth, however their magnitudes show a reasonable agreement with other contemporary observations. Both the original and recalibration datasets are being submitted to PANGAEA data repository for its storage and public access. [ABSTRACT FROM AUTHOR]

Nitric Acid Trihydrate (NAT) crystal formation in the absence of water ice is important for a subset of Polar Stratospheric Clouds (PSCs) and thereby ozone depletion. It has been suggested that either fragmented meteoroids or meteoric smoke particles (MSPs), or possibly both, are important as heterogeneous nuclei of these crystals. Previous work has focused on the nucleating ability of meteoric material in nitric acid in the absence of sulfuric acid. However, it is known that when immersed in stratospheric sulfuric acid droplets, metal-containing meteoric material particles partially dissolve and components can re-precipitate as silica and alumina that have different morphologies to the original meteoric material. Hence, in this study we experimentally and theoretically explore the relative role that sulfuric acid-processed meteoric smoke and meteoric fragments may play in NAT nucleation in PSCs. We compared meteoric fragments that had been recently prepared (by milling a meteorite sample) to a sample annealed under conditions designed to simulate heating during entry into the Earth's atmosphere. Whilst the addition of sulfuric acid decreased the nucleating ability of the recently milled meteoric material relative to nucleation in binary nitric acid-water solutions (at similar NAT saturation ratio), the annealed meteoric fragments nucleated NAT with a similar effectiveness in both solutions. However, combining our results with measured fluxes of meteoric material to the Earth, sedimentation modelling and recent experiments on fragmentation of incoming meteoroids, suggests that there are unlikely to be sufficient fragments to contribute to the nucleation of crystalline NAT particles. We then considered silica formed from sulfuric acid processed meteoric smoke particles. Our previous work showed that nanoparticulate silica (radius ~6 nm) is a relatively poor promoter of nucleation compared with micron scaled silica particles, which were more effective. Both materials have similar chemical and structural (crystallographically amorphous) properties, indicating size is critical. Here we account for surface curvature of primary grains using Classical Nucleation Theory (CNT) to explore this size dependence. This model is able to explain the discrepancy in nucleation effectiveness of fumed silica and fused quartz, by treating their nucleating activity (contact angle) as equal but with differing particle size (or surface curvature), assuming interfacial energies that are physically reasonable. Here we use this CNT model to present evidence that nucleation of NAT on acid processed MSPs, where the primary grain size is 10s nm, is also effective enough to contribute to NAT crystals in early season PSCs where there is an absence of ice. This study demonstrates that modelling of crystal nucleation in PSCs and resulting ozone depletion relies on accurate understanding of the transport and chemical processing of MSPs. This will affect estimated sensitivity of stratospheric chemistry to rare events such as large volcanic eruptions and long-term forecasting of ozone recovery in a changing climate. [ABSTRACT FROM AUTHOR]

Recent model inter-comparison studies highlighted model discrepancies in reproducing the climatic impacts of large explosive volcanic eruptions, calling into question the reliability of global aerosol model simulations for future scenarios. Here, we analyse the simulated evolution of the stratospheric aerosol plume following the well observed June 1991 Mt. Pinatubo eruption by six interactive stratospheric aerosol microphysics models in comparison to a range of observational data sets. Our primary focus 5 is on the uncertainties regarding initial SO2 emission following the Pinatubo eruption in 1991, as prescribed in the Historical Eruptions SO2 Emission Assessment experiments (HErSEA), in the framework of the Interactive Stratospheric Aerosol Model Intercomparison Project (ISA-MIP). Six global models with interactive aerosol microphysics took part in this study: ECHAM6-SALSA, EMAC, ECHAM5-HAM, SOCOL-AERv2, ULAQ-CCM and UM-UKCA. Model simulations are performed by varying SO2 injection amount (ranging between 5 and 10 Tg-S), and the altitude of injection (between 18-25 km). We find that the common and main weakness among all the models is that they can not reproduce the persistence of the sulfate aerosols in the stratosphere. Most models show a stronger transport towards the extratropics in the northern hemisphere, at the expense of the observed tropical confinement, suggesting a much weaker subtropical barrier in all the models, that results in a shorter e-folding time compared to the observations. Moreover, the simulations in which more than 5 Tg-S of SO2 are injected show a large surface area density a few months after the eruption compared to the values measured in the tropics and the in-situ measurements over Laramie. This results in an overestimation of the number of particles globally during the build-up phase and an underestimation in the Southern Hemisphere, which draws attention to the importance of including processes as the ash injection and the eruption of Cerro Hudson. [ABSTRACT FROM AUTHOR]

This paper provides initial results from a multi-model ensemble analysis based on the volc-pinatubo-full experiment performed within the Model Intercomparison Project on the climatic response to Volcanic forcing (VolMIP) as part of the sixth phase of the Coupled Model Intercomparison Project (CMIP6). The volc-pinatubo-full experiment is based on an ensemble of volcanic forcing-only climate simulations with the same volcanic aerosol dataset across the participating models (the 1991–1993 Pinatubo period from the CMIP6-GloSSAC dataset). The simulations are conducted within an idealized experimental design where initial states are sampled consistently across models from the CMIP6-piControl simulation providing unperturbed preindustrial background conditions. The multi-model ensemble includes output from an initial set of six participating Earth system models (CanESM5, GISS-E2.1-G, IPSL-CM6A-LR, MIROC-E2SL, MPI-ESM1.2-LR and UKESM1). The results show overall good agreement between the different models on the global and hemispheric scales concerning the surface climate responses, thus demonstrating the overall effectiveness of VolMIP's experimental design. However, small yet significant inter-model discrepancies are found in radiative fluxes, especially in the tropics, that preliminary analyses link with minor differences in forcing implementation; model physics, notably aerosol–radiation interactions; the simulation and sampling of El Niño–Southern Oscillation (ENSO); and, possibly, the simulation of climate feedbacks operating in the tropics. We discuss the volc-pinatubo-full protocol and highlight the advantages of volcanic forcing experiments defined within a carefully designed protocol with respect to emerging modelling approaches based on large ensemble transient simulations. We identify how the VolMIP strategy could be improved in future phases of the initiative to ensure a cleaner sampling protocol with greater focus on the evolving state of ENSO in the pre-eruption period. [ABSTRACT FROM AUTHOR]

Until now our understanding of the 11-year solar cycle signal (SCS) in stratospheric ozone has been largely based on high-quality but sparse ozone profiles from the Stratospheric Aerosol and Gas Experiment (SAGE) II or coarsely resolved ozone profiles from the nadir-viewing Solar Backscatter Ultraviolet Radiometer (SBUV) satellite instruments. Here, we analyse 16 years (2005–2020) of ozone profile measurements from the Microwave Limb Sounder (MLS) instrument on the Aura satellite to estimate the 11-year SCS in stratospheric ozone. Our analysis of Aura-MLS data suggests a single-peak-structured SCS profile (about 3 % near 4 hPa or 40 km) in tropical stratospheric ozone, which is significantly different to the SAGE II and SBUV-based double-peak-structured SCS. We also find that MLS-observed ozone variations are more consistent with ozone from our control model simulation that uses Naval Research Laboratory (NRL) v2 solar fluxes. However, in the lowermost stratosphere modelled ozone shows a negligible SCS compared to about 1 % in Aura-MLS data. An ensemble of ordinary least squares (OLS) and three regularised (lasso, ridge and elastic net) linear regression models confirms the robustness of the estimated SCS. In addition, our analysis of MLS and model simulations shows a large SCS in the Antarctic lower stratosphere that was not seen in earlier studies. We also analyse chemical transport model simulations with alternative solar flux data. We find that in the upper (and middle) stratosphere the model simulation with Solar Radiation and Climate Experiment (SORCE) satellite solar fluxes is also consistent with the MLS-derived SCS and agrees well with the control simulation and one which uses Spectral and Total Irradiance Reconstructions (SATIRE) solar fluxes. Hence, our model simulation suggests that with recent adjustments and corrections, SORCE data can be used to analyse effects of solar flux variations. Furthermore, analysis of a simulation with fixed solar fluxes and one with fixed (annually repeating) meteorology confirms that the implicit dynamical SCS in the (re)analysis data used to force the model is not enough to simulate the observed SCS in the middle and upper stratospheric ozone. Finally, we argue that the overall significantly different SCS compared to previous estimates might be due to a combination of different factors such as much denser MLS measurements, almost linear stratospheric chlorine loading changes over the analysis period, variations in the stratospheric dynamics as well as relatively unperturbed stratospheric aerosol layer that might have influenced earlier analyses. [ABSTRACT FROM AUTHOR]

This paper provides initial results from a multi-model ensemble analysis based on the volc-pinatubo-full experiment performed within the Model Intercomparison Project on the climatic response to volcanic forcing (VolMIP) as part of the sixth phase of the Coupled Model Intercomparison Project (CMIP6). The volc-pinatubo-full experiment is based on ensemble of volcanic forcing-only climate simulations with the same volcanic aerosol dataset across the participating models (the 1991-1993 Pinatubo period from the CMIP6-GloSSAC dataset). The simulations are conducted within an idealized experimental design where initial states are sampled consistently across models from the CMIP6-piControl simulation providing unperturbed pre-industrial background conditions. The multi-model ensemble includes output from an initial set of six participating Earth system models (CanESM5, GISS-E2.1-G, IPSL-CM6A-LR, MIROC-E2SL, MPI-ESM1.2-LR and UKESM1). The results show overall good agreement between the different models on the global and hemispheric scale concerning the surface climate responses, thus demonstrating the overall effectiveness of VolMIP's experimental design. However, small yet significant inter-model discrepancies are found in radiative fluxes especially in the tropics, that preliminary analyses link with minor differences in forcing implementation, model physics, notably aerosol-radiation interactions, the simulation and sampling of El Niño-Southern Oscillation (ENSO) and, possibly, the simulation of climate feedbacks operating in the tropics. We discuss the volc-pinatubo-full protocol and highlight the advantages of volcanic forcing experiments defined within a carefully designed protocol with respect to emerging modeling approaches based on large ensemble transient simulations. We identify how the VolMIP strategy could be improved in future phases of the initiative to ensure a cleaner sampling protocol with greater focus on the evolving state of ENSO in the pre-eruption period. [ABSTRACT FROM AUTHOR]

We report the recovery and processing methodology of the first ever multi-year lidar dataset of the stratospheric aerosol layer. A Q-switched ruby lidar measured 66 vertical profiles of 694 nm attenuated backscatter at Lexington, Massachusetts, between January 1964 and August 1965, with an additional nine profile measurements conducted from College, Alaska, during July and August 1964. We describe the processing of the recovered lidar backscattering ratio profiles to produce mid-visible (532 nm) stratospheric aerosol extinction profiles (sAEP 532) and stratospheric aerosol optical depth (sAOD 532) measurements, utilizing a number of contemporary measurements of several different atmospheric variables. Stratospheric soundings of temperature and pressure generate an accurate local molecular backscattering profile, with nearby ozone soundings determining the ozone absorption, which are used to correct for two-way ozone transmittance. Two-way aerosol transmittance corrections are also applied based on nearby observations of total aerosol optical depth (across the troposphere and stratosphere) from sun photometer measurements. We show that accounting for these two-way transmittance effects substantially increases the magnitude of the 1964/1965 stratospheric aerosol layer's optical thickness in the Northern Hemisphere mid-latitudes, then ∼ 50 % larger than represented in the Coupled Model Intercomparison Project 6 (CMIP6) volcanic forcing dataset. Compared to the uncorrected dataset, the combined transmittance correction increases the sAOD 532 by up to 66 % for Lexington and up to 27 % for Fairbanks, as well as individual sAEP 532 adjustments of similar magnitude. Comparisons with the few contemporary measurements available show better agreement with the corrected two-way transmittance values. Within the January 1964 to August 1965 measurement time span, the corrected Lexington sAOD 532 time series is substantially above 0.05 in three distinct periods, October 1964, March 1965, and May–June 1965, whereas the 6 nights the lidar measured in December 1964 and January 1965 had sAOD values of at most ∼ 0.03. The comparison with interactive stratospheric aerosol model simulations of the Agung aerosol cloud shows that, although substantial variation in mid-latitude sAOD 532 are expected from the seasonal cycle in the stratospheric circulation, the Agung cloud's dispersion from the tropics would have been at its strongest in winter and weakest in summer. The increasing trend in sAOD from January to July 1965, also considering the large variability, suggests that the observed variations are from a different source than Agung, possibly from one or both of the two eruptions that occurred in 1964/1965 with a Volcanic Explosivity Index (VEI) of 3: Trident, Alaska, and Vestmannaeyjar, Heimaey, south of Iceland. A detailed error analysis of the uncertainties in each of the variables involved in the processing chain was conducted. Relative errors for the uncorrected sAEP 532 were 54 % for Fairbanks and 44 % Lexington. For the corrected sAEP 532 the errors were 61 % and 64 %, respectively. The analysis of the uncertainties identified variables that with additional data recovery and reprocessing could reduce these relative error levels. Data described in this work are available at 10.1594/PANGAEA.922105 (Antuña-Marrero et al., 2020a). [ABSTRACT FROM AUTHOR]

Until now our understanding of the 11-year solar cycle signal (SCS) in stratospheric ozone has been largely based on high quality but sparse ozone profiles from the Stratospheric Aerosol and Gas Experiment (SAGE) II or coarsely resolved ozone profiles from the nadir-viewing Solar Backscatter Ultraviolet Radiometer (SBUV) satellite instruments. Here, we analyse 16 years (2005-2020) of ozone profile measurements from the Microwave Limb Sounder (MLS) instrument on the Aura satellite to estimate the 11-year SCS in stratospheric ozone. Our analysis of Aura-MLS data suggests a single-peak-structured SCS profile (about 3% near 4 hPa or 40 km) in tropical stratospheric ozone, which is significantly different to the SAGE II and SBUV-based double-peak-structured SCS. We also find that MLS-observed ozone variations are more consistent with ozone from our control model simulation that uses Naval Research Laboratory (NRL) v2 solar fluxes. However, in the lowermost stratosphere modelled ozone shows a negligible SCS compared to about 1% in Aura-MLS data. An ensemble of Ordinary Least Square (OLS) and three regularised (Lasso, Ridge and ElasticNet) linear regression models confirms the robustness of the estimated SCS. Our analysis of MLS and model simulations also shows a large SCS in the Antarctic lower stratosphere that was not seen in earlier studies. We also analyse chemical transport model simulations with alternative solar flux data. We find that in the upper (and middle) stratosphere the model simulation with Solar Radiation and Climate Experiment (SORCE) satellite solar fluxes is also consistent with the MLS-derived SCS and agrees well with the control simulation and one which uses Spectral and Total Irradiance Reconstructions (SATIRE) solar fluxes. Hence, our model simulation suggests that with recent adjustments and corrections, SORCE solar fluxes can be used to analyse effects of solar flux variations. Finally, we argue that the overall significantly different SCS compared to earlier estimates might be due to a combination of different factors such as much denser MLS measurements, almost linear stratospheric chlorine loading changes over the analysis period, as well as a stratospheric aerosol layer relatively unperturbed by major volcanic eruptions. [ABSTRACT FROM AUTHOR]

As part of the Model Intercomparison Project on the climatic response to Volcanic forcing (VolMIP), several climate modeling centers performed a coordinated pre-study experiment with interactive stratospheric aerosol models simulating the volcanic aerosol cloud from an eruption resembling the 1815 Mt. Tambora eruption (VolMIP-Tambora ISA ensemble). The pre-study provided the ancillary ability to assess intermodel diversity in the radiative forcing for a large stratospheric-injecting equatorial eruption when the volcanic aerosol cloud is simulated interactively. An initial analysis of the VolMIP-Tambora ISA ensemble showed large disparities between models in the stratospheric global mean aerosol optical depth (AOD). In this study, we now show that stratospheric global mean AOD differences among the participating models are primarily due to differences in aerosol size, which we track here by effective radius. We identify specific physical and chemical processes that are missing in some models and/or parameterized differently between models, which are together causing the differences in effective radius. In particular, our analysis indicates that interactively tracking hydroxyl radical (OH) chemistry following a large volcanic injection of sulfur dioxide (SO2) is an important factor in allowing for the timescale for sulfate formation to be properly simulated. In addition, depending on the timescale of sulfate formation, there can be a large difference in effective radius and subsequently AOD that results from whether the SO2 is injected in a single model grid cell near the location of the volcanic eruption, or whether it is injected as a longitudinally averaged band around the Earth. [ABSTRACT FROM AUTHOR]

We report the recovery and processing methodology of the first ever multi-year lidar dataset of the stratospheric aerosol layer. A Q-switched Ruby lidar measured 66 vertical profiles of 694nm attenuated backscatter at Lexington, Massachusetts between January 1964 and August 1965, with an additional 9 profile measurements conducted from College, Alaska during July and August 1964. We describe the processing of the recovered lidar backscattering ratio profiles to produce mid-visible (532nm) stratospheric aerosol extinction profiles (sAEP532) and stratospheric aerosol optical depth (sAOD532) measurements, utilizing a number of contemporary measurements of several different atmospheric variables. Stratospheric soundings of temperature, and pressure generate an accurate local molecular backscattering profile, with nearby ozone soundings determining the ozone absorption, those profiles then used to correct for two-way ozone transmittance. Two-way aerosol transmittance corrections were also applied based on nearby observations of total aerosol optical depth (across the troposphere and stratosphere) from sun photometer measurements . We show the two-way transmittance correction has substantial effects on the retrieved sAEP532 and sAOD532, calculated without the corrections resulting in substantially lower values of both variables, as it was not applied in the original processing producing the lid ar scattering ratio profiles we rescued. The combined transmittance corrections causes the aerosol extinction to increase by 67 % for Lexington and 27 % for Fairbanks, for sAOD532 the increases 66 % and 26 % respectively. Comparing the magnitudes of the aerosol extinction and sAOD with the few contemporary available measurements reported show a better agreement in the case of the two way transmittance corrected values. The sAEP and sAOD timeseries at Lexington show a surprisingly large degree of variability, three periods where the stratospheric aerosol layer had suddenly elevated optical thickness, the highest sAOD532 of 0.07 measured at the end of March 1965. The two other periods of enhanced sAOD532 are both two-month periods where the lidars show more than 1 night where ret rieved sAOD532 exceeded 0.05: in January and February 1964 and November and December 1964. Interactive stratospheric aerosol model simulations of the 1963 Agung cloud illustrate that although substantial variation in mid-latitude sAOD532 is expected from the seasonal cycle in the Brewer-Dobson circulation, the Agung cloud dispersion will have caused much slower increase than the more episodic variations observed, with also different timing, elevated optical thickness from Agung occurring in winter and spring. The abruptness and timing of the steadily increasing sAOD from January to July 1965 suggests this variation was from a different source than Agung, possibly from one or both of the two VEI3 eruptions that occurred in 1964/65: Trident, Alaska and Vestmannaeyjar, Heimey, south of Iceland. A detailed error analysis of the uncertainties in each of the variables involved in the processing chain was conducted, relative errors of 54 % for Fairbanks and 44 % Lexington for the uncorrected sAEP532, corrected sAEP532 of 61 % and 64 % respectively. The analysis of the uncertainties identified variables that, with additional data recovery and reprocessing could reduce these relative error levels. Data described in this work are available at https://doi.pangaea.de/10.1594/PANGAEA.922105 (Dataset in Review) (Antuña-Marrero et al., 2020a). [ABSTRACT FROM AUTHOR]

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); , and) 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. [ABSTRACT FROM AUTHOR]

A key limitation of volcanic forcing datasets for the Pinatubo period is the large uncertainty that remains with respect to the extent of the optical depth of the Pinatubo aerosol cloud in the first year after the eruption, the saturation of the SAGE-II instrument restricting it to only be able to measure the upper part of the aerosol cloud in the tropics. Here we report the recovery of stratospheric aerosol measurements from two shipborne lidars, both of which measured the tropical reservoir of volcanic aerosol produced by the June 1991 Mount Pinatubo eruption. The lidars were on board two Soviet vessels, each ship crossing the Atlantic, their measurement datasets providing unique observational transects of the Pinatubo cloud across the tropics from Europe to the Caribbean (∼ 40 to 8 ∘ N) from July to September 1991 (the Professor Zubov ship) and from Europe to south of the Equator (∼ 40 ∘ N to 8 ∘ S) between January and February 1992 (the Professor Vize ship). Our philosophy with the data recovery is to follow the same algorithms and parameters that appear in the two peer-reviewed articles that presented these datasets in the same issue of GRL in 1993, and here we provide all 48 lidar soundings made from the Professor Zubov and 11 of the 20 conducted from the Professor Vize , ensuring we have reproduced the aerosol backscatter and extinction values in the figures of those two papers. These original approaches used thermodynamic properties from the CIRA-86 standard atmosphere to derive the molecular backscattering, vertically and temporally constant values applied for the aerosol backscatter-to-extinction ratio, and the correction factor of the aerosol backscatter wavelength dependence. We demonstrate this initial validation of the recovered stratospheric aerosol extinction profiles, providing full details of each dataset in this paper's Supplement S1, the original profiles of backscatter ratio, and the calculated profiles of aerosol backscatter and extinction. We anticipate these datasets will provide potentially important new observational case studies for modelling analyses, including a 1-week series of consecutive soundings (in September 1991) at the same location showing the progression of the entrainment of part of the Pinatubo plume into the upper troposphere and the formation of an associated cirrus cloud. The Zubov lidar dataset illustrates how the tropically confined Pinatubo aerosol cloud transformed from a highly heterogeneous vertical structure in August 1991, maximum aerosol extinction values around 19 km for the lower layer and 23–24 for the upper layer, to a more homogeneous and deeper reservoir of volcanic aerosol in September 1991. We encourage modelling groups to consider new analyses of the Pinatubo cloud, comparing the recovered datasets, with the potential to increase our understanding of the evolution of the Pinatubo aerosol cloud and its effects. Data described in this work are available at 10.1594/PANGAEA.912770 (Antuña-Marrero et al., 2020). [ABSTRACT FROM AUTHOR]

As part of the Model Intercomparison Project on the climatic response to Volcanic forcing (VolMIP), several climate modeling centers performed a coordinated pre-study experiment with interactive stratospheric aerosol models simulating the volcanic aerosol cloud from an eruption resembling the 1815 Mt Tambora eruption (VolMIP-Tambora ISA ensemble). The pre-study provided the ancillary ability to assess intermodel diversity in the radiative forcing for a large stratospheric-injecting equatorial eruption when the volcanic aerosol cloud is simulated interactively. An initial analysis of the VolMIP-Tambora ISA ensemble showed large disparities between models in the stratospheric global mean aerosol optical depth (AOD). In this study, we now show that stratospheric global mean AOD differences among the participating models are primarily due to differences in aerosol size, which we track here by effective radius. We identify specific physical and chemical processes that are missing in some models and/or parameterized differently between models, which are together causing the differences in effective radius. In particular, our analysis indicates that interactively tracking hydroxyl radical (OH) chemistry following a large volcanic injection of sulfur dioxide (SO2) is an important factor in allowing for the timescale for sulfate formation to be properly simulated. In addition, depending on the timescale of sulfate formation, there can be a large difference in effective radius and subsequently AOD that results from whether the SO2 is injected in a single model gridcell near the location of the volcanic eruption, or whether it is injected as a longitudinally averaged band around the Earth. [ABSTRACT FROM AUTHOR]

A key limitation of volcanic forcing datasets for the Pinatubo period, is the large uncertainty that remains with respect to the extent of the optical depth of the Pinatubo aerosol cloud in the first year after the eruption, the saturation of the SAGE-II instrument restricting it to only be able to measure the upper part of the aerosol cloud in the tropics. Here we report the recovery of stratospheric aerosol measurements from two ship-borne lidars, both of which measured the tropical reservoir of volcanic aerosol produced by the June 1991 Mount Pinatubo eruption. The lidars were on-board two Soviet vessels, each ship crossing the Atlantic, their measurement datasets providing unique observational transects of the Pinatubo cloud across the tropics from Europe to the Caribbean (~ 40° N to 8° N) from July to September 1991 (the Prof Zubov ship) and from Europe to south of the Equator (8° S to ~ 40° N) between January and February 1992 (the Prof Vizeship). Our philosophy with the data recovery is to follow the same algorithms and parameters appearing in the two peer-reviewed articles that presented these datasets in the same issue of GRL in 1993, and here we provide all 48 lidar soundings made from the Prof. Zubov, and 11 of the 20 conducted from the Prof. Vize, ensuring we have reproduced the aerosols backscatter and extinction values in the Figures of those two papers. These original approaches used thermodynamic properties from the CIRA-86 standard atmosphere to derive the molecular backscattering, vertically and temporally constant values applied for the aerosol backscatter to extinction ratio and the correction factor of the aerosols backscattering wavelength dependence. We demonstrate this initial validation of the recovered stratospheric aerosol extinction profiles, providing full details of each dataset in this paper's Supplement S1, the original text files of the backscatter ratio, the calculated aerosols backscatter and extinction profiles. We anticipate the data providing potential new observational case studies for modelling analyses, including a 1-week series of consecutive soundings (in September 1991) at the same location showing the progression of the entrainment of part of the Pinatubo plume into the upper troposphere and the formation of an associated cirrus cloud. The Zubov lidar dataset illustrates how the tropically confined Pinatubo aerosol cloud transformed from a highly heterogeneous vertical structure in August 1991, maximum aerosol extinction values around 19 km for the lower layer and 23-24 for the upper layer, to a more homogeneous and deeper reservoir of volcanic aerosol in September 1991. We encourage modelling groups to consider new analyses of the Pinatubo cloud, comparing to the recovered datasets, with the potential to increase our understanding of the evolution of the Pinatubo aerosol cloud and its effects. Data described in this work are available at https://doi.pangaea.de/10.1594/PANGAEA.912770 (Antuña-Marrero et al., 2020). [ABSTRACT FROM AUTHOR]

Accurate quantification of the effects of volcanic eruptions on climate is a key requirement for better attribution of anthropogenic climate change. Here we use the UM-UKCA composition-climate model to simulate the atmospheric evolution of the volcanic aerosol clouds from the three largest eruptions of the 20th century: 1963 Agung, 1982 El Chichón and 1991 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 3-member ensemble model experiments with upper, mid-point and lower estimates for SO2 emission, each initialised to a meteorological state to match the observed phase of the quasi-biennial oscillation (QBO) at the times of the eruptions. We assess how each eruption's emitted SO2 evolves into a tropical reservoir of volcanic aerosol and analyse the subsequent dispersion to mid-latitudes. We compare the simulations to the three volcanic forcing datasets used in historical integrations for the two most recent Coupled Model Intercomparison Project (CMIP) assessments: the Global Space-based Stratospheric Aerosol Climatology (GloSSAC) for CMIP6, and the Sato et al. (1993) and Ammann et al. (2003) datasets used in CMIP5. We also assess the vertical extent of the volcanic aerosol clouds by comparing simulated extinction to Stratospheric Aerosol and Gas Experiment II (SAGE-II) v7.0 satellite aerosol data (1985-1995) for Pinatubo and El Chichón, and to 1964-65 northern hemisphere ground-based lidar measurements for Agung. As an independent test for the simulated volcanic forcing after Pinatubo, we also compare to the shortwave (SW) and longwave (LW) Top-of-the-Atmosphere 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 sulphur burden, with good agreement also to SAGE-II mid-visible and near-infrared extinction measurements. This 10-14 Tg range of emission also generates a heating of the tropical stratosphere that is comparable with the temperature anomaly seen in the ERA-Interim reanalyses. For El Chichón the simulations with 5 Tg and 7 Tg SO2 emission give best agreement with the observations. However, these runs predict a much deeper volcanic cloud than present in the CMIP6 data, with much higher aerosol extinction than the GloSSAC data up to October 1984, but better agreement during the later SAGE-II period. For 1963 Agung, the 9 Tg simulation compares best to the forcing datasets with the model capturing the lidar-observed signature of peak extinction descending from 20 km in 1964 to 16 km in 1965. Overall, our results indicate that the downward adjustment to previous SO2 emission estimates for Pinatubo as suggested by several interactive modelling studies is also needed for the Agung and El Chichón aerosol clouds. This strengthens the hypothesis that interactive stratospheric aerosol models may be missing an important removal or redistribution 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 analysis identifies potentially important inhomogeneities in the CMIP6 dataset for all three periods that are hard to reconcile with variations predicted by the interactive stratospheric aerosol model. 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. [ABSTRACT FROM AUTHOR]

The representation of volatile organic compound (VOC) deposition and oxidation mechanisms in the context of secondary organic aerosol (SOA) formation are developed in the United Kingdom Chemistry and Aerosol (UKCA) chemistry–climate model. Impacts of these developments on both the global SOA budget and model agreement with observations are quantified. Firstly, global model simulations were performed with varying VOC dry deposition and wet deposition fluxes. Including VOC dry deposition reduces the global annual-total SOA production rate by 2 %–32 %, with the range reflecting uncertainties in surface resistances. Including VOC wet deposition reduces the global annual-total SOA production rate by 15 % and is relatively insensitive to changes in effective Henry's law coefficients. Without precursor deposition, simulated SOA concentrations are lower than observed with a normalised mean bias (NMB) of -51 %. Hence, including SOA precursor deposition worsens model agreement with observations even further (NMB =-66 %). Secondly, for the anthropogenic and biomass burning VOC precursors of SOA (VOC ANT/BB), model simulations were performed by (a) varying the parent hydrocarbon reactivity, (b) varying the number of reaction intermediates, and (c) accounting for differences in volatility between oxidation products from various pathways. These changes were compared to a scheme where VOC ANT/BB adopts the reactivity of a monoterpene (α -pinene), and is oxidised in a single-step mechanism with a fixed SOA yield. By using the chemical reactivity of either benzene, toluene, or naphthalene for VOC ANT/BB , the global annual-total VOC ANT/BB oxidation rate changes by -3 %, -31 %, or -66 %, respectively, compared to when using α -pinene. Increasing the number of reaction intermediates, by introducing a peroxy radical (RO2), slightly slows the rate of SOA formation, but has no impact on the global annual-total SOA production rate. However, RO2 undergoes competitive oxidation reactions, forming products with substantially different volatilities. Accounting for the differences in product volatility between RO2 oxidation pathways increases the global SOA production rate by 153 % compared to using a single SOA yield. Overall, for relatively reactive compounds such as toluene and naphthalene, the reduction in reactivity for VOC ANT/BB oxidation is outweighed by accounting for the difference in volatility of RO2 products, leading to a net increase in the global annual-total SOA production rate of 85 % and 145 %, respectively, and improvements in model agreement (NMB of -46 % and 56 %, respectively). However, for benzene, the reduction in VOC ANT/BB oxidation is not outweighed by accounting for the difference in SOA yield pathways, leading to a small change in the global annual-total SOA production rate of -3 %, and a slight worsening of model agreement with observations (NMB =-77 %). These results highlight that variations in both VOC deposition and oxidation mechanisms contribute to substantial uncertainties in the global SOA budget and model agreement with observations. [ABSTRACT FROM AUTHOR]

The Stratospheric Sulfur and its Role in Climate (SSiRC) Interactive Stratospheric Aerosol Model Intercomparison Project (ISA-MIP) explores uncertainties in the processes that connect volcanic emission of sulfur gas species and the radiative forcing associated with the resulting enhancement of the stratospheric aerosol layer. The central aim of ISA-MIP is to constrain and improve interactive stratospheric aerosol models and reduce uncertainties in the stratospheric aerosol forcing by comparing results of standardized model experiments with a range of observations. In this paper we present four co-ordinated inter-model experiments designed to investigate key processes which influence the formation and temporal development of stratospheric aerosol in different time periods of the observational record. The Background (BG) experiment will focus on microphysics and transport processes under volcanically quiescent conditions, when the stratospheric aerosol is controlled by the transport of aerosols and their precursors from the troposphere to the stratosphere. The Transient Aerosol Record (TAR) experiment will explore the role of small- to moderate-magnitude volcanic eruptions, anthropogenic sulfur emissions, and transport processes over the period 1998-2012 and their role in the warming hiatus. Two further experiments will investigate the stratospheric sulfate aerosol evolution after major volcanic eruptions. The Historical Eruptions SO2 Emission Assessment (HErSEA) experiment will focus on the uncertainty in the initial emission of recent large-magnitude volcanic eruptions, while the Pinatubo Emulation in Multiple models (PoEMS) experiment will provide a comprehensive uncertainty analysis of the radiative forcing from the 1991 Mt Pinatubo eruption. [ABSTRACT FROM AUTHOR]

The representation of volatile organic compound (VOC) deposition and oxidation mechanisms in the context of secondary organic aerosol (SOA) formation are developed in the United Kingdom Chemistry and Aerosol (UKCA) chemistry-climate model. Impacts of these developments on both the global SOA budget and model agreement with observations is quantified. Firstly, global model simulations were performed with varying VOC dry deposition and wet deposition. Including VOC dry deposition reduces the global annual-total SOA production rate by 2-32 %, with the range reflecting uncertainties in surface resistances. Including VOC wet deposition reduces the global annual-total SOA production rate by 15 % and is relatively insensitive to changes in effective Henry's Law coefficients. With precursor deposition, simulated SOA concentrations are lower than observed, with a normalised mean bias (NMB) of -51 %. Hence, including SOA precursor deposition worsens model agreement with observations even further (NMB = -66 %). Secondly, for the anthropogenic and biomass burning VOC precursors of SOA (VOCANT/BB), model simulations were performed varying: a) the parent hydrocarbon reactivity, b) the number of reaction intermediates, and c) accounting for differences in volatility between oxidation products from various pathways. These changes were compared to a scheme where VOCANT/BB adopts the reactivity of monoterpene (α-pinene), and is oxidised in a single-step mechanism with a fixed SOA yield. By using the chemical reactivity of either benzene, toluene or naphthalene for VOCANT/BB, the global annual-total VOCANT/BB oxidation rate changes by -3, -31 or -66 %, respectively, compared to when using monoterpene. Increasing the number of reaction intermediates, by introducing a peroxy radical (RO2), slightly slows the rate of SOA formation, but has no impact on the global annual-total SOA production rate. However, RO2 undergoes competitive oxidation reactions, forming products with substantially different volatilities. Accounting for the differences in product volatility between RO2 oxidation pathways increases the global SOA production rate by 153 % compared to using a single SOA yield. Overall, for relatively reactive compounds, such as toluene and naphthalene, the reduction in reactivity for VOCANT/BB oxidation is outweighed by accounting for the difference in volatility of RO2 products, leading to a net increase in the global annual-total SOA production rate of 85 and 145 %, respectively, and improvemtns in model agreement (NMB of -46 and 56 %, respectively). However, for benzene, the reduction in VOCANT/BB oxidation is not outweighed by accounting for the difference in SOA yield pathways, leading to a small change in the global annual-total SOA production rate of -3 %, and a slight worsening of model agreement with observatiobs (NMB = -77 %). These results highlight that variations in both VOC deposition and oxidation mechanisms contribute to substantial uncertainties in the global SOA budget and model agreement with observations. [ABSTRACT FROM AUTHOR]

The global secondary organic aerosol (SOA) budget is highly uncertain, with global annual SOA production rates, estimated from global models, ranging over an order of magnitude and simulated SOA concentrations underestimated compared to observations. In this study, we use a global composition-climate model (UKCA) with interactive chemistry and aerosol microphysics to provide an indepth analysis of the impact of each VOC source on the global SOA budget and its seasonality. We further quantify the role of each source on SOA spatial distributions, and evaluate simulated seasonal SOA concentrations against a comprehensive set of observations. The annual global SOA production rates from monoterpene, isoprene, biomass burning, and anthropogenic precursor sources is 19.9, 19.6, 9.5, and 24.6 Tg.SOA/ a-1, respectively. When all sources are included, the SOA production rate from all sources is 73.6 Tg.SOA/ a-1, which lies within the range of estimates from previous modelling studies. SOA production rates and SOA burdens from biogenic and biomass burning SOA sources peak during Northern Hemisphere (NH) summer. In contrast, the anthropogenic SOA production rate is fairly constant all year round. However, the global anthropogenic SOA burden does have a seasonal cycle which is lowest during NH summer, which is probably due to enhanced wet removal. Inclusion of the new SOA sources also accelerates the ageing by condensation of primary organic aerosol (POA), making it more hydrophilic, leading to a reduction in the POA lifetime. With monoterpene as the only source of SOA, simulated SOA and total organic aerosol (OA) concentrations are underestimated by the model when compared to surface and aircraft measurements. Model agreement with observations improves with all new sources added, primarily due to the inclusion of the anthropogenic source of SOA, although a negative bias remains. A further sensitivity simulation was performed with an increased anthropogenic SOA reaction yield, corresponding to an annual global SOA production rate of 70.0 Tg.SOA/ a-1. Whilst simulated SOA concentrations improved relative to observations, they were still underestimated in urban environments and overestimated further downwind and in remote environments. In contrast, the inclusion of SOA from isoprene and biomass burning did not improve model--observations biases substantially except at one out of two tropical locations. However, these findings may reflect the very limited availability of observations to evaluate the model, which are primarily located in the NH mid-latitudes where anthropogenic emissions are high. Our results highlight that, within the current uncertainty limits in SOA sources and reaction yields, over the NH mid-latitudes, a large anthropogenic SOA source results in good agreement with observations. However, more observations are needed to establish the importance of biomass burning and biogenic sources of SOA in model agreement with observations. [ABSTRACT FROM AUTHOR]

The eruption of Mt. Tambora in 1815 was the largest volcanic eruption of the past 500 years. The eruption had significant climatic impacts, leading to the 1816 year without a summer, and remains a valuable event from which to understand the climatic effects of large stratospheric volcanic sulfur dioxide injections. The eruption also resulted in one of the strongest and most easily identifiable volcanic sulfate signals in polar ice cores, which are widely used to reconstruct the timing and atmospheric sulfate loading of past eruptions. As part of the Model Intercomparison Project on the climatic response to Volcanic forcing (VolMIP), five state-of-the-art global aerosol models simulated this eruption. We analyse both simulated background (no Tambora) and volcanic (with Tambora) sulfate deposition to polar regions and compare to ice core records. The models simulate overall similar patterns of background sulfate deposition, although there are differences in regional details and magnitude. However, the volcanic sulfate deposition varies considerably between the models with differences in timing, spatial pattern and magnitude. Mean simulated deposited sulfate on Antarctica ranges from 19 to 264 kg km−2 and on Greenland from 31 to 194 kg km−2, as compared to the mean ice-core-derived estimates of roughly 50 kg km−2 for both Greenland and Antarctica. The ratio of the hemispheric atmospheric sulfate aerosol burden after the eruption to the average ice sheet deposited sulfate varies between models by up to a factor of 15. Sources of this inter-model variability include differences in both the formation and the transport of sulfate aerosol. Our results suggest that deriving relationships between sulfate deposited on ice sheets and atmospheric sulfate burdens from model simulations may be associated with greater uncertainties than previously thought. [ABSTRACT FROM AUTHOR]

The global secondary organic aerosol (SOA) budget is highly uncertain, with global annual SOA production rates, estimated from global models, ranging over an order of magnitude and simulated SOA concentrations underestimated compared to observations. In this study, we use a global composition-climate model (UKCA) with interactive chemistry and aerosol microphysics to provide an in-depth analysis of the impact of each SOA source on the global SOA budget and its seasonality. We further quantify the role of each source on SOA spatial distributions, and evaluate simulated seasonal SOA concentrations against a comprehensive set of observations. The annual global SOA production rates from monoterpene, isoprene, biomass burning and anthropogenic precursor sources is 19.9 19.6, 9.5 and 24.6 Tg (SOA) a-1 respectively. When all sources are included, the SOA production rate from all sources is 73.6 Tg (SOA) a-1, which lies within the range of estimates from previous modelling studies. SOA production rates and SOA burdens from biogenic and biomass burning SOA sources peak during northern hemisphere (NH) summer. In contrast, the an thropogenic SOA production rate is fairly constant all year round. However, the global anthropogenic SOA burden does have a seasonal cycle which is lowest during NH summer, which is probably due to enhanced wet removal. Inclusion of the new SOA sources also accelerates the ageing by condensation of primary organic aerosol (POA), making it more hydrophilic, leading to a reduction in the POA lifetime. With monoterpene as the only source of SOA, simulated SOA and total organic aerosol (OA) concentrations are underestimated by the model when compared to surface and aircraft measurements. Model agreement with observations improves with all new sources added, primarily due to the inclusion of the anthropogenic source of SOA, although a negative bias remains. A further sensitivity simulation was performed with an increased anthropogenic SOA reaction yield, corresponding to an annual global SOA production rate of 70.0 Tg (SOA) a-1. Whilst simulated SOA concentrations improved relative to observations, they were still underestimated in urban environments and overestimated further downwind and in remote environments respectively. On the other hand, the inclusion of SOA from isoprene and biomass burning did not improve model-observations biases substantially except at one out of two tropical locations. However, these findings may reflect the very limited availability of observations to evaluate the model, which are primarily located in the NH mid-latitudes where anthropogenic emissions are high. Our results highlight that, within the current uncertainty limits in SOA sources and reaction yields, over the NH mid-latitudes, a large anthropogenic SOA source results in good agreement with observations. However, more observations are needed to establish the importance of biomass burning and biogenic sources of SOA in model agreement with observations. [ABSTRACT FROM AUTHOR]

The eruption of Mt. Tambora in 1815 was the largest volcanic eruption of the past 500 years. The eruption had significant climatic impacts, leading to the 1816 Year Without a Summer and remains a valuable event from which to understand the climatic effects of large stratospheric volcanic sulfur dioxide injections. The eruption also resulted in one of the strongest and most easily identifiable volcanic signals in polar ice cores, which are widely used to reconstruct the timing and atmospheric sulfate loading of past eruptions. As part of the Model Intercomparison Project on the climatic response to Volcanic forcing (VolMIP), four state-of-the-art global aerosol models simulated this eruption. We analyse both simulated background (no Tambora) and volcanic (with Tambora) sulfate deposition to polar regions and compare to ice core records. Background sulfate deposition is of similar magnitude across all models and compares well to ice core records. However, volcanic sulfate deposition varies in timing, spatial pattern and magnitude between the models. Mean simulated deposited sulfate on Antarctica ranges from 19 to 264 kg km-2, and on Greenland from 31 to 194 kg km-2, as compared to the mean ice core-derived estimates of roughly 40-50 kg km-2, for both Greenland and Antarctica. The ratio of the hemispheric atmospheric sulfate aerosol burden after the eruption to the average ice sheet deposited sulfate varies between models by up to a factor of 15. Sources of this inter-model variability include differences in both the formation and the transport of sulfate aerosol. Our results highlight the uncertainties and difficulties in deriving historic volcanic aerosol radiative forcing of climate, based on measured volcanic sulfate in polar ice cores. [ABSTRACT FROM AUTHOR]

A convection-permitting limited area model with periodic lateral boundary conditions and prognostic aerosol microphysics is applied to investigate how concentrations of cloud condensation nuclei (CCN) in the marine boundary layer are affected by high-resolution dynamical and thermodynamic fields. The high-resolution aerosol microphysics-dynamics model, which resolves differential particle growth and aerosol composition across the particle size range, is applied to a domain designed to match approximately a single grid square of a climate model. We find that, during strongly convective conditions with high wind-speed conditions, CCN concentrations vary by more than a factor of 8 across the domain (5-95th percentile range), and a factor of ~3 at more moderate wind speed. One reason for these large subclimate-grid-scale variations in CCN is that emissions of sea salt and dimethyl sulfide (DMS) are much higher when spatial and temporal wind-speed fluctuations become resolved at this convection-permitting resolution (making peak wind speeds higher). By analysing how the model evolves during spin-up, we gain new insight into the way primary sea salt and secondary sulfate particles contribute to the overall CCN variance in these realistic conditions, and find a marked difference in the variability of super-micron and sub-micron CCN. Whereas the super-micron CCN are highly variable, dominated by strongly fluctuating sea spray emitted, the submicron CCN tend to be steadier, mainly produced on longer timescales following growth after new particle formation in the free troposphere, with fluctuations inherently buffered by the fact that coagulation is faster at higher particle concentrations. We also find that sub-micron CCN are less variable in particle size, the accumulation-mode mean size varying by ~20% (0.101 to 0.123 μm diameter) compared to ~35% (0.75 to 1.10 μm diameter) for coarse-mode particles at this resolution. We explore how the CCN variability changes in the vertical and at different points in the spin-up, showing how CCN concentrations are introduced both by the emissions close to the surface and at higher altitudes during strong wind-speed conditions associated to the intense convective period. We also explore how the non-linear variation of seasalt emissions with wind speed propagates into variations in sea-salt mass mixing ratio and CCN concentrations, finding less variation in the latter two quantities due to the longer transport timescales inherent with finer CCN, which sediment more slowly. The complex mix of sources and diverse community of processes involved makes sub-grid parameterisation of CCN variations difficult. However, the results presented here illustrate the limitations of predictions with large-scale models and the high-resolution aerosol microphysics-dynamics modelling system shows promise for future studies where the aerosol variations will propagate through to modified cloud microphysical evolution. [ABSTRACT FROM AUTHOR]

We present observations of biomass burning aerosol from the South American Biomass Burning Analysis (SAMBBA) and other measurement campaigns, and use these to evaluate the representation of biomass burning aerosol properties and processes in a state-of-the-art climate model. The evaluation includes detailed comparisons with aircraft and ground data, along with remote sensing observations from MODIS and AERONET. We demonstrate several improvements to aerosol properties following the implementation of the Global Model for Aerosol Processes (GLOMAP-mode) modal aerosol scheme in the HadGEM3 climate model. This predicts the particle size distribution, composition, and optical properties, giving increased accuracy in the representation of aerosol properties and physical-chemical processes over the Coupled Largescale Aerosol Scheme for Simulations in Climate Models (CLASSIC) bulk aerosol scheme previously used in HadGEM2. Although both models give similar regional distributions of carbonaceous aerosol mass and aerosol optical depth (AOD), GLOMAP-mode is better able to capture the observed size distribution, single scattering albedo, and Ångström exponent across different tropical biomass burning source regions. Both aerosol schemes overestimate the uptake of water compared to recent observations, CLASSIC more so than GLOMAP-mode, leading to a likely overestimation of aerosol scattering, AOD, and single scattering albedo at high relative humidity. Observed aerosol vertical distributions were well captured when biomass burning aerosol emissions were injected uniformly from the surface to 3 km. Finally, good agreement between observed and modelled AOD was gained only after scaling up GFED3 emissions by a factor of 1.6 for CLASSIC and 2.0 for GLOMAPmode. We attribute this difference in scaling factor mainly to different assumptions for the water uptake and growth of aerosol mass during ageing via oxidation and condensation of organics. We also note that similar agreement with observed AOD could have been achieved with lower scaling factors if the ratio of organic carbon to primary organic matter was increased in the models toward the upper range of observed values. Improved knowledge from measurements is required to reduce uncertainties in emission ratios for black carbon and organic carbon, and the ratio of organic carbon to primary organic matter for primary emissions from biomass burning. [ABSTRACT FROM AUTHOR]

The dissolution of semi-volatile inorganic gases such as ammonia and nitric acid into the aerosol aqueous phase has an important influence on the composition, hygroscopic properties, and size distribution of atmospheric aerosol particles. The representation of dissolution in global models is challenging due to inherent issues of numerical stability and computational expense. For this reason, simplified approaches are often taken, with many models treating dissolution as an equilibrium process. In this paper we describe the new dissolution solver HyDiS-1.0, which was developed for the global size-resolved simulation of aerosol inorganic composition. The solver applies a hybrid approach, which allows for some particle size classes to establish instantaneous gas-particle equilibrium, whereas others are treated time dependently (or dynamically). Numerical accuracy at a competitive computational expense is achieved by using several tailored numerical formalisms and decision criteria, such as for the time- and size-dependent choice between the equilibrium and dynamic approaches. The new hybrid solver is shown to have numerical stability across a wide range of numerical stiffness conditions encountered within the atmosphere. For ammonia and nitric acid, HyDiS-1.0 is found to be in excellent agreement with a fully dynamic benchmark solver. In the presence of sea salt aerosol, a somewhat larger bias is found under highly polluted conditions if hydrochloric acid is represented as a third semi-volatile species. We present first results of the solver's implementation into a global aerosol microphysics and chemistry transport model. We find that (1) the new solver predicts surface concentrations of nitrate and ammonium in reasonable agreement with observations over Europe, the USA, and East Asia, (2) models that assume gas-particle equilibrium will not capture the partitioning of nitric acid and ammonia into Aitken-mode-sized particles, and thus may be missing an important pathway through which secondary particles may grow to radiation- and cloudinteracting size, and (3) the new hybrid solver's computational expense is modest, at around 10%of total computation time in these simulations. [ABSTRACT FROM AUTHOR]

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 ∼ 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. [ABSTRACT FROM AUTHOR]

The enhancement of the stratospheric aerosol layer by volcanic eruptions induces a complex set of responses causing global and regional climate effects on a broad range of timescales. Uncertainties exist regarding the climatic response to strong volcanic forcing identified in coupled climate simulations that contributed to the fifth phase of the Coupled Model Intercomparison Project (CMIP5). In order to better understand the sources of these model diversities, the Model Intercomparison Project on the climatic response to Volcanic forcing (VolMIP) has defined a coordinated set of idealized volcanic perturbation experiments to be carried out in alignment with the CMIP6 protocol. VolMIP provides a common stratospheric aerosol data set for each experiment to minimize differences in the applied volcanic forcing. It defines a set of initial conditions to assess how internal climate variability contributes to determining the response. VolMIP will assess to what extent volcanically forced responses of the coupled ocean-atmosphere system are robustly simulated by state-of-the-art coupled climate models and identify the causes that limit robust simulated behavior, especially differences in the treatment of physical processes. This paper illustrates the design of the idealized volcanic perturbation experiments in the VolMIP protocol and describes the common aerosol forcing input data sets to be used. [ABSTRACT FROM AUTHOR]

The vertical profile of aerosol is important for its radiative effects, but weakly constrained by observations on the global scale, and highly variable among different models. To investigate the controlling factors in one particular model, we investigate the effects of individual processes in HadGEM3-UKCA and compare the resulting diversity of aerosol vertical profiles with the inter-model diversity from the AeroCom Phase II control experiment. In this way we show that (in this model at least) the vertical profile is controlled by a relatively small number of processes, although these vary among aerosol components and particle sizes. We also show that sufficiently coarse variations in these processes can produce a similar diversity to that among different models in terms of the global-mean profile and, to a lesser extent, the zonal-mean vertical position. However, there are features of certain models' profiles that cannot be reproduced, suggesting the influence of further structural differences between models. In HadGEM3-UKCA, convective transport is found to be very important in controlling the vertical profile of all aerosol components by mass. In-cloud scavenging is very important for all except mineral dust. Growth by condensation is important for sulfate and carbonaceous aerosol (along with aqueous oxidation for the former and ageing by soluble material for the latter). The vertical extent of biomass-burning emissions into the free troposphere is also important for the profile of carbonaceous aerosol. Boundary-layer mixing plays a dominant role for sea salt and mineral dust, which are emitted only from the surface. Dry deposition and below-cloud scavenging are important for the profile of mineral dust only. In this model, the microphysical processes of nucleation, condensation and coagulation dominate the vertical profile of the smallest particles by number (e.g. total CN >3 nm), while the profiles of larger particles (e.g. CN>100 nm) are controlled by the same processes as the component mass profiles, plus the size distribution of primary emissions. We also show that the processes that affect the AODnormalised radiative forcing in the model are predominantly those that affect the vertical mass distribution, in particular convective transport, in-cloud scavenging, aqueous oxidation, ageing and the vertical extent of biomass-burning emissions. [ABSTRACT FROM AUTHOR]

The dissolution of semi-volatile inorganic gases such as ammonia and nitric acid into the aerosol liquid phase has an important influence on the composition, hygroscopic properties and size distribution of atmospheric aerosol particles. The representation of dissolution in global models is challenging due to inherent issues of numerical stability and computational expense. For this reason, simplified approaches are often taken, with many models treating dissolution as an equilibrium process. In this paper we describe the new dissolution solver HyDiS-1.0 that was developped for the global size-resolved simulation of aerosol inorganic composition. The solver applies a hybrid approach, which allows some particle size increments to establish instantaneous gas-particle equilibrium while others are treated time dependently (or dynamically). Numerical accuracy at a competitive computational expense is achieved by using several tailored numerical formalisms and decision criteria, such as for the time- and size-dependent choice between the equilibrium and dynamic approaches. The new hybrid solver is shown to be in good to excellent agreement with a fully dynamic solver and to have numerical stability across a wide range of numerical stiffness conditions encountered within the atmosphere. We present first results of the solver's implementation into a global aerosol microphysics and chemistry transport model. We find that (1) the new solver predicts surface concentrations of nitrate and ammonium in reasonable agreement with observations over Europe, the US and East Asia; (2) models that assume gas-particle equilibrium will not capture the partitioning of nitric acid and ammonia into Aitken mode sized particles, and thus may be missing an important pathway whereby secondary particles may grow to radiation and cloud-interacting size; and (3) the new hybrid solver's computational expense is modest, at around 10 % of total computation time in these simulations. [ABSTRACT FROM AUTHOR]

We revisit the original SAGE-II and lidar gap-filling volcanic aerosol datasets in the initial months following the Pinatubo eruption. During that period, the lower stratosphere was so optically opaque making impossible for SAGE II to conduct reliable measurements. We make use of five lidar datasets for that period we have compiled from research teams. None of these datasets were used for gap filling in the most recent stratospheric aerosols climatology. The Aspendale ground-based lidar measurements in the southern hemisphere were made throughout the 2nd half of 1991, also measuring the depolarization of the plume from early 1992. Two ship-borne lidar from the Russian vessels Prof. Zubov ship Atlantic transect from Europe to the Caribbean July to September 1991 and Prof. Vize ship transect from Europe to south of the Equator between January and February 1992. Two NASA airborne lidar missions. NASA-Electra Aircraft Missions to the Caribbean on July 12, 13 and 14 1991 and NASA-Ames Aircraft Mission to the Pacific to the Pacific on May 24 and 26 1992. We present preliminary analysis of these datasets and will combine them with ensemble of simulations with the UM-UKCA interactive stratospheric aerosol model and identify best fit to the measurements retaining also the fine-scale spatial and temporal evolution of the volcanic aerosol cloud. The activity aligns with a new "data rescue" activity in the 2nd phase of the SPARC initiative "Stratospheric Sulphur and its Role in Climate" (SSiRC). We will make the lidar datasets available to the scientific community in a public repository via the SSiRC website. [ABSTRACT FROM AUTHOR]

The widespread presence of meteoric smoke particles (MSPs) within a distinct class of stratospheric aerosol particles has become clear from in-situ measurements in the Arctic, Antarctic and at mid-latitudes. Knowledge of how extensive inclusions of MSPs occur within the liquid background stratospheric aerosol is important in light of growing evidence that many polar stratospheric clouds form heterogeneously in the Arctic. In this study, we first explain the adaptation of the interactive stratosphere-troposphere aerosol-chemistry-climate model UM-UKCA to additionally resolve the heterogeneous nucleation of meteoric-sulphuric particles, alongside the existing pure aqueous sulphuric acid particles formed by homogeneous nucleation.We present the simulated global distribution of both types of stratospheric aerosol particle showing how they form on 10-20nm MSP cores in the uppermost stratospheric aerosol layer at high latitudes, as MSPs are transported down from the mesosphere within the polar vortex. Our simulations suggest that meteoric-sulphuric particles contribute around 5-10 particles per cc additional condensation nuclei to the upper half of the winter polar stratospheric aerosol layer at particle sizes around 30-70nm. Although the meteoric-sulphuric particles are at lower concentrations in the mid-latitude stratosphere, resolving their presence in the model changes dramatically the simulated lifecyle of the background pure stratospheric sulphuric particles. The additional condensation sink from the MSP-core particles reduces the condensational growth of the pure sulphuric particles, changing their vertical distribution, stratospheric residence time and transport trajectory within the prevailing Brewer-Dobson circulation. We find that resolving both sulphuric particle types in the model reduces the simulated stratospheric aerosol layer sulphur burden by a factor of 5 and greatly improves CN concentration predictions, remedying a previous high bias in the upper stratospheric aerosol layer from excessive particle formation in polar winter and spring. Comparing to particle concentration measurements at Laramie, our results suggest that, aside from the observed layer of enhanced concentrations (at 30km) during late winter early spring (which is caused by homogeneous particle formation), in other months, the vertical profile of CN (Dp>10nm) is approximately constant above 20km, the change from the decreasing profile from 15-20km caused both by the MSP-nucleated sulphuric particles and a strong additional seasonal variation (absent in previous simulations) caused by meridional transport of pure sulphuric particles homogeneous nucleated in the tropics. [ABSTRACT FROM AUTHOR]

The Stratospheric Sulfur and its Role in Climate (SSiRC) interactive stratospheric aerosol model intercomparison project (ISA-MIP) explores uncertainties in the processes that connect volcanic emission of sulphur gas species and the radiative forcing associated with the resulting enhancement of the stratospheric aerosol layer. The central aim of ISA-MIP is to constrain and improve interactive stratospheric aerosol models and reduce uncertainties in the stratospheric aerosol forcing by comparing results of standardized model experiments with a range of observations. In this paper we present 4 co-ordinated inter-model experiments designed to investigate key processes which influence the formation and temporal development of stratospheric aerosol in different time periods of the observational record. The "Background" (BG) experiment will focus on microphysics and transport processes under volcanically quiescent conditions, when the stratospheric aerosol is controlled by the transport of aerosols and their precursors from the troposphere to the stratosphere. The "Transient Aerosol Record" (TAR) experiment will explore the role of small- to moderate-magnitude volcanic eruptions, anthropogenic sulphur emissions and transport processes over the period 1998-2012 and their role in the warming hiatus. Two further experiments will investigate the stratospheric sulphate aerosol evolution after major volcanic eruptions. The "Historical Eruptions SO2 Emission Assessment" (HErSEA) experiment will focus on the uncertainty in the initial emission of recent large-magnitude volcanic eruptions, while the "Pinatubo Emulation in Multiple models" (PoEMS) experiment will provide a comprehensive uncertainty analysis of the radiative forcing from the 1991 Mt. Pinatubo eruption. [ABSTRACT FROM AUTHOR]