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The recovery and re-calibration of a dataset of vertical aerosol extinction profiles of the 1963/64 stratospheric aerosol layer measured by a searchlight at 32° N in New Mexico, US, is reported. The recovered dataset consists of 105 aerosol extinction profiles at 550 nm that cover the period from December 1963 to December 1964. It is a unique record of the portion of the aerosol cloud from the March 1963 Agung volcanic eruption that was transported into the Northern Hemisphere subtropics. The data-recovery methodology involved re-digitizing the 105 original aerosol extinction profiles from individual Figures within a research report, followed by the re-calibration. It involves inverting the original equation used to compute the aerosol extinction profile to retrieve the corresponding normalized detector response profile. The re-calibration of the original aerosol extinction profiles used Rayleigh extinction profiles calculated from local soundings. Rayleigh and aerosol slant transmission corrections are applied using the MODTRAN code in transmission mode. Also, a best-estimate aerosol phase function was calculated from observations and applied to the entire column. The tropospheric aerosol phase function from an AERONET station in the vicinity of the searchlight location was applied between 2.76 to 11.7 km. The stratospheric phase function, applied for a 12.2 to 35.2 km altitude range, is calculated from particle-size distributions measured by a high-altitude aircraft in the vicinity of the searchlight in early 1964. The original error estimate was updated considering unaccounted errors. Both the re-calibrated aerosol extinction profiles and the re-calibrated stratospheric aerosol optical depth magnitudes showed higher magnitudes than the original aerosol extinction profiles and the original stratospheric aerosol optical depth, respectively. However, the magnitudes of the re-calibrated variables show a reasonable agreement with other contemporary observations. The re-calibrated stratospheric aerosol optical depth demonstrated its consistency with the tropics-to-pole decreasing trend, associated with the major volcanic eruption stratospheric aerosol pattern when compared to the time-coincident stratospheric aerosol optical depth lidar observations at Lexington at 42° N. [ABSTRACT FROM AUTHOR]

​​​​​​​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]

The January 2022 eruption of Hunga Tonga‐Hunga Ha'apai (HTHH) injected a huge amount (∼150 Tg) of water vapor (H2O) into the stratosphere, along with small amount of SO2. An off‐line 3‐D chemical transport model (CTM) successfully reproduces the spread of the injected H2O through October 2023 as observed by the Microwave Limb Sounder. Dehydration in the 2023 Antarctic polar vortex caused the first substantial (∼20 Tg) removal of HTHH H2O from the stratosphere. The CTM indicates that this process will dominate removal of HTHH H2O for the coming years, giving an overall e‐folding timescale of 4 years; around 25 Tg of the injected H2O is predicted to still remain in the stratosphere by 2030. Following relatively low Antarctic column ozone in midwinter 2023 due to transport effects, additional springtime depletion due to H2O‐related chemistry was small and maximized at the vortex edge (10 DU in column). Plain Language Summary: Around 150 Tg (150 million tons) of water vapor was injected into the stratosphere during the eruption of Hunga Tonga‐Hunga Ha'apai. Water vapor is a greenhouse gas and this increase is expected to have a warming effect in the troposphere, as well causing perturbations in stratospheric chemistry and aerosols. We use an atmospheric model to study the residence time of this excess water vapor and its impact on the recent Antarctic ozone hole. The model performance is evaluated by comparison with satellite measurements. Wintertime dehydration in the Antarctic stratosphere in 2023 is found to be an important mechanism for removal of the volcanic water from the stratosphere. However, the overall removal rate is predicted to be slow; around 25 Tg (17%) is still present in 2030. The direct impact of the excess water vapor on ozone via chemical processes in the Antarctic ozone hole in 2023 is small. Key Points: Antarctic dehydration is a major removal pathway of stratospheric H2O injected from Hunga Tonga‐Hunga Ha'apai (HTHH) eruptionHTHH H2O caused small (up to 10 DU) additional chemical ozone depletion in 2023 Antarctic springModel indicates e‐folding timescale of 4 years for removal of HTHH H2O from stratosphere [ABSTRACT FROM AUTHOR]

Substantial and prolonged enhancements in stratospheric water vapor (SWV) have occurred after large‐magnitude explosive tropical volcanic eruptions, with modified tropopause entry caused by aerosol‐absorptive heating. Here, we analyze the timing and longevity of heating‐driven post‐eruption SWV changes within CMIP6‐VolMIP short‐term climate‐response experiments with the UK Earth System Model (UKESM1). We find aerosol‐absorptive heating causes peak SWV increases of 17% (∼1 ppmv) and 10% (0.5 ppmv) at 100 and 50 hPa, at ∼18 and ∼23 months after a Pinatubo‐like eruption, respectively. We track the temperature response in the tropical lower stratosphere and identify the main SWV increase occurs only after the descending aerosol heating reaches the tropopause, suggesting a key role for aerosol microphysical processes (sedimentation rate). We explore how El Niño–Southern Oscillation variability modulates this effect. Post‐eruption SWV increases are ∼80% stronger for the La Nina phase compared to the ensemble mean. Tropical upwelling strongly mediates this effect. Plain Language Summary: Strong volcanic eruptions, such as the 1991 eruption of Mt Pinatubo, inject a large amount of SO2 directly into the stratosphere, thereby enhancing the stratospheric aerosol layer and causing a short‐term climatic perturbation. Another substantial part of the climatic influence is the change in stratospheric water vapor (SWV), which affects the chemical processes and the radiative budget of the atmosphere. Along with near‐instantaneous injection of water vapor into the stratosphere, volcanic eruptions can indirectly enhance the entry of water vapor into the stratosphere through aerosol‐induced tropopause heating. This work analyses Earth system model experiments designed to explore how volcanic impacts combine with internal climate variability. We find that peak SWV entry mixing ratios occur only within the second post‐eruption year, consistent with the substantially lagged timing of SWV increase seen in post‐Pinatubo satellite measurements. This analysis provides a new perspective on the temporal evolution of the observed post‐Pinatubo SWV increase and an improved quantification of its impacts. Key Points: Aerosol‐induced absorptive‐heating increases stratospheric water vapor (SWV) by up to 17% at 18 months post‐eruption in a Pinatubo‐like experimentAnalyzing simulations by El Niño–Southern Oscillation (ENSO) variability show an 80% larger peak SWV increase occurs if an eruption is followed by a La Niña phaseThe timing of peak SWV increase occurs when volcanic‐aerosol‐induced heating reaches the tropopause, with ENSO modulation of tropical upwelling [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]

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]

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]

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]

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]

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]

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 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]

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]