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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]

Aerosols have a potentially large effect on climate, particularly through their interactions with clouds, but the magnitude of this effect is highly uncertain. Large volcanic eruptions produce sulfur dioxide, which in turn produces aerosols; these eruptions thus represent a natural experiment through which to quantify aerosolcloud interactions. Here we show that the massive 20142015 fissure eruption in Holuhraun, Iceland, reduced the size of liquid cloud dropletsconsistent with expectationsbut had no discernible effect on other cloud properties. The reduction in droplet size led to cloud brightening and global-mean radiative forcing of around 0.2 watts per square metre for September to October 2014. Changes in cloud amount or cloud liquid water path, however, were undetectable, indicating that these indirect effects, and cloud systems in general, are well buffered against aerosol changes. This result will reduce uncertainties in future climate projections, because we are now able to reject results from climate models with an excessive liquid-water-path response., Author(s): Florent F. Malavelle (corresponding author) [1]; Jim M. Haywood [1, 2]; Andy Jones [2]; Andrew Gettelman [3]; Lieven Clarisse [4]; Sophie Bauduin [4]; Richard P. Allan [5, 6]; Inger [...]

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]

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]

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]

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]

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]

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]