Sulfur Injection Research Articles

No Evidence of Winter Warming in Eurasia Following Large, Low-Latitude Volcanic Eruptions during the Last Millennium

Abstract We critically reexamine the question of whether volcanic eruptions cause surface warming over Eurasia in winter, in the light of recent modeling studies that have suggested internal variability may overwhelm any forced volcanic response, even for the very largest eruptions during the Common Era. Focusing on the last millennium, we combine model output, instrumental observations, tree-ring records, and ice cores to build a new temperature reconstruction that specifically targets the boreal winter season. We focus on 20 eruptions over the last millennium with volcanic stratospheric sulfur injections (VSSIs) larger than the 1991 Pinatubo eruption. We find that only 7 of these 20 large events are followed by warm surface temperature anomalies over Eurasia in the first posteruption winter. Examining the 13 events that show cold posteruption anomalies, we find no correlation between the amplitude of winter cooling and VSSI mass. We also find no evidence that the North Atlantic Oscillation is correlated with VSSI in winter, a key element of the proposed mechanism through which large, low-latitude eruptions might cause winter warming over Eurasia. Furthermore, by inspecting individual eruptions rather than combining events into a superposed epoch analysis, we are able to reconcile our findings with those of previous studies. Analysis of two additional paleoclimatic datasets corroborates the lack of posteruption Eurasian winter warming. Our findings, covering the entire last millennium, confirm the findings of most recent modeling studies and offer important new evidence that large, low-latitude eruptions are not, in general, followed by significant surface wintertime warming over Eurasia.

Extreme Tibetan Plateau cooling caused by tropical volcanism

The extreme cooling of the Tibetan Plateau (TP) during the boreal winter typically poses threats to the local environment and people’s safety, and it is usually attributed to internal climate variability. Here we demonstrate that the five recent large tropical volcanic eruptions since 1880 have caused an average extreme cooling of up to −0.80 K on the TP in observations during the first boreal winter following the eruptions. This cooling effect is much larger than the global average terrestrial cooling of −0.30 K after the eruptions. The multi-model ensemble mean (MME) of the Atmospheric Model Intercomparison Project (AMIP) runs from Phase 6 of the Coupled Model Intercomparison Project (CMIP6), in which realistic sea surface temperatures (SST) were specified, can simulate an extreme TP cooling response of up to −0.79 K, which is much larger than the direct aerosol cooling of −0.36 K simulated by the historical runs. The positive North Atlantic Oscillation (NAO) anomaly during the post-eruption winter after the eruptions plays a key role in amplifying the TP cooling through atmospheric teleconnection, which overwhelms the warming response associated with the frequently occurring El Niños. The results from this study provide a perspective on the potential contribution of volcanic activity or stratospheric sulfur injection scenarios to specific TP cooling.

Dependency of the impacts of geoengineering on the stratospheric sulfur injection strategy – Part 2: How changes in the hydrological cycle depend on the injection rate and model used

Abstract. This is the second of two papers in which we study the dependency of the impacts of stratospheric sulfur injections on the model and injection strategy used. Here, aerosol optical properties from simulated stratospheric aerosol injections using two aerosol models (modal scheme M7 and sectional scheme SALSA), as described in Part 1 (Laakso et al., 2022), are implemented consistently into the EC-Earth, MPI-ESM and CESM Earth system models (ESMs) to simulate the climate impacts of different injection rates ranging from 2 to 100 Tg(S) yr−1. Two sets of simulations were run with the three ESMs: (1) regression simulations, in which an abrupt change in CO2 concentration or stratospheric aerosols over pre-industrial conditions was applied to quantify global mean fast temperature-independent climate responses and quasi-linear dependence on temperature, and (2) equilibrium simulations, in which radiative forcing of aerosol injections with various magnitudes compensated for the corresponding radiative forcing of CO2 enhancement to study the dependence of precipitation on the injection magnitude. The latter also allow one to explore the regional climatic responses. Large differences in SALSA- and M7-simulated radiative forcing in Part 1 translated into large differences in the estimated surface temperature and precipitation changes in ESM simulations; for example, an injection rate of 20 Tg(S) yr−1 in CESM using M7-simulated aerosols led to only 2.2 K global mean cooling, while EC-Earth–SALSA combination produced a 5.2 K change. In equilibrium simulations, where aerosol injections were utilized to offset the radiative forcing caused by an atmospheric CO2 concentration of 500 ppm, the decrease in global mean precipitation varied among models, ranging from −0.7 % to −2.4 % compared with the pre-industrial climate. These precipitation changes can be explained by the fast precipitation response due to radiation changes caused by the stratospheric aerosols and CO2, as the global mean fast precipitation response is shown to be negatively correlated with global mean atmospheric absorption. Our study shows that estimating the impact of stratospheric aerosol injection on climate is not straightforward. This is because the simulated capability of the sulfate layer to reflect solar radiation and absorb long-wave radiation is sensitive to the injection rate as well as the aerosol model used to simulate the aerosol field. These findings emphasize the necessity for precise simulation of aerosol microphysics to accurately estimate the climate impacts of stratospheric sulfur intervention. This study also reveals gaps in our understanding and uncertainties that still exist related to these controversial techniques.

Fine quantitative characterization of high-H2S gas reservoirs under the influence of liquid sulfur deposition and adsorption

In order to clarify the influence of liquid sulfur deposition and adsorption to high-H2S gas reservoirs, three types of natural cores with typical carbonate pore structures were selected for high-temperature and high-pressure core displacement experiments. Fine quantitative characterization of the cores in three steady states (original, after sulfur injection, and after gas flooding) was carried out using the nuclear magnetic resonance (NMR) transverse relaxation time spectrum and imaging, X-ray computer tomography (CT) of full-diameter cores, basic physical property testing, and field emission scanning electron microscopy imaging. The loss of pore volume caused by sulfur deposition and adsorption mainly comes from the medium and large pores with sizes bigger than 1 000 μm. Liquid sulfur has a stronger adsorption and deposition ability in smaller pore spaces, and causes greater damage to reservoirs with poor original pore structures. The pore structure of the three types of carbonate reservoirs shows multiple fractal characteristics. The worse the pore structure, the greater the change of internal pore distribution caused by liquid sulfur deposition and adsorption, and the stronger the heterogeneity. Liquid sulfur deposition and adsorption change the pore size distribution, pore connectivity, and heterogeneity of the rock, which further changes the physical properties of the reservoir. After sulfur injection and gas flooding, the permeability of Type I reservoirs with good physical properties decreased by 16%, and that of Types II and III reservoirs with poor physical properties decreased by 90% or more, suggesting an extremely high damage. This indicates that the worse the initial physical properties, the greater the damage of liquid sulfur deposition and adsorption. Liquid sulfur is adsorbed and deposited in different types of pore space in the forms of flocculence, cobweb, or retinitis, causing different changes in the pore structure and physical property of the reservoir.

Description and performance of a sectional aerosol microphysical model in the Community Earth System Model (CESM2)

Abstract. We implemented the Community Aerosol and Radiation Model for Atmospheres (CARMA) in both the high- and low-top model versions of the Community Earth System Model Version 2 (CESM2). CARMA is a sectional microphysical model, which we use for aerosol in both the troposphere and stratosphere. CARMA is fully coupled to chemistry, clouds, radiation, and transport routines in CESM2. This development enables the comparison of simulations with a sectional (CARMA) and a modal (MAM4) aerosol microphysical model in the same modeling framework. The new implementation of CARMA has been adopted from previous work, with some additions that align with the current CESM2 Modal Aerosol Model (MAM4) implementation. The main updates include an interactive secondary organic aerosol description in CARMA, using the volatility basis set (VBS) approach, updated wet removal, and the use of transient emissions of aerosols and trace gases. In addition, we implemented an alternative aerosol nucleation scheme in CARMA, which is also used in MAM4. Detailed comparisons of stratospheric aerosol properties after the Mount Pinatubo eruption reveal the importance of prescribing sulfur injections in a larger region rather than in a single column to better represent the observed evolution of aerosols. Both CARMA and MAM4 in CESM2 are able to represent stratospheric and tropospheric aerosol properties reasonably well when compared to observations. Several differences in the performance of the two aerosol models show, in general, an improved representation of aerosols when using the sectional aerosol model in CESM2. These include a better representation of the aerosol size distribution after the Mount Pinatubo volcanic eruption in CARMA compared to MAM4. MAM4 produces on average smaller aerosols and less removal than CARMA, which results in a larger total mass. Both CARMA and MAM4 reproduce the stratospheric aerosol optical depth (AOD) within the error bar of the observations between 2001 and 2020, except for recent larger volcanic eruptions that are overestimated by both model configurations. The CARMA background surface area density and aerosol size distribution in the stratosphere and troposphere compare well to observations, with some underestimation of the Aitken-mode size range. MAM4 shows shortcomings in reproducing coarse-mode aerosol distributions in the stratosphere and troposphere. This work outlines additional development needs for CESM2 CARMA to improve the model compared to observations in both the troposphere and stratosphere.

A New Multi‐Method Assessment of Stratospheric Sulfur Load From the Okmok II Caldera‐Forming Eruption of 43 BCE

AbstractThe 43 BCE eruption of Okmok Volcano has been proposed to have had a significant climate cooling impact in the Northern Hemisphere. In this study, we quantify the climate cooling potential of the Okmok II eruption by measuring sulfur concentration in melt inclusions (up to 1,606 ppm) and matrix glasses and estimate a total of 62 ± 16 Tg S released. The proportion reaching the stratosphere (2.5%–25%, i.e., 1.5–15.5 Tg S) was constrained by physical modeling of the caldera‐collapse eruption. Using the NASA Goddard Institute for Space Studies E2.2 climate model we found a linear response between cooling and stratospheric sulfur load (0.05–0.08°C/Tg S). Thus, the 1–2°C of cooling derived from proxy records would require 16–32 Tg sulfur injection. This study underscores the importance of combining approaches to estimate stratospheric S load. For Okmok II, we find all methods are consistent with a range of 15–16 Tg S.

A Bimetallic Organic Framework with Mn in MIL-101(Cr) for Lithium-Sulfur Batteries.

Lithium-sulfur batteries (LSBs) show excellent performance in terms of specific capacity and energy density. However, the cyclic stability of LSBs is compromised due to the "shuttle effect", which hinders the practical applications of LSBs. Herein, a metal-organic framework (MOF) based on Cr ions as the main body composition, commonly known as MIL-101(Cr), was utilized to minimize the shuttle effect and improve the cyclic performance of LSBs. To obtain MOFs with a certain adsorption capacity for lithium polysulfide and a certain catalytic capacity, we propose an effective strategy of incorporating sulfur-loving metal ions (Mn) into the skeleton to enhance the reaction kinetics at the electrode. Based on the oxidation doping method, Mn2+ was uniformly dispersed in MIL-101(Cr) to produce bimetallic Cr2O3/MnOx as a novel sulfur-carrying cathode material. Then, a sulfur injection process was carried out by melt diffusion to obtain the sulfur-containing Cr2O3/MnOx-S electrode. Moreover, an LSB assembled with Cr2O3/MnOx-S showed improved first-cycle discharge (1285 mAh·g-1 at 0.1 C) and cyclic performance (721 mAh·g-1 at 0.1 C after 100 cycles), and the overall performance was much better than that of monometallic MIL-101(Cr) as a sulfur carrier. These results revealed that the physical immobilization method of MIL-101(Cr) positively affected the adsorption of polysulfides, while the bimetallic composite Cr2O3/MnOx formed by the doping of sulfur-loving Mn2+ into the porous MOF produced a good catalytic effect during LSB charging. This research provides a novel approach for preparing efficient sulfur-containing materials for LSBs.

The effect of uncertainties in natural forcing records on simulated temperature during the last millennium

Abstract. Here we investigate how uncertainties in the solar and volcanic forcing records of the past millennium affect the large-scale temperature response using a two-box impulse response model. We use different published solar forcing records and present a new volcanic forcing ensemble that accounts for random uncertainties in eruption dating and sulfur injection amount. The simulations are compared to proxy reconstructions from PAGES 2k and Northern Hemispheric tree ring data. We find that low solar forcing is most consistent with all the proxy reconstructions, even when accounting for volcanic uncertainty. We also find that the residuals are in line with CMIP6 control variability at centennial timescales. Volcanic forcing uncertainty induces a significant spread in the temperature response, especially at periods of peak forcing. For individual eruptions and superposed epoch analyses, volcanic uncertainty can strongly affect the agreement with proxy reconstructions and partly explain known proxy–model discrepancies.

Reconstructing volcanic radiative forcing since 1990, using a comprehensive emission inventory and spatially resolved sulfur injections from satellite data in a chemistry-climate model

Abstract. This paper presents model simulations of stratospheric aerosols with a focus on explosive volcanic eruptions. Using various (occultation and limb-based) satellite instruments, providing vertical profiles of sulfur dioxide (SO2) and aerosol extinction, we characterized the chemical and radiative influence of volcanic aerosols for the period between 1990 and 2019. We established an improved and extended volcanic SO2 emission inventory that includes more than 500 explosive volcanic eruptions reaching the upper troposphere and the stratosphere. Each perturbation identified was derived from the satellite data and incorporated as a three-dimensional SO2 plume into a chemistry-climate model without the need for additional assumptions about altitude distribution and eruption duration as needed for a “point source” approach. The simultaneous measurements of SO2 and aerosol extinction by up to four satellite instruments enabled a reliable conversion of extinction measurements into injected SO2. In the chemistry-climate model, the SO2 from each individual plume was converted into aerosol particles and their optical properties were determined. Furthermore, the aerosol optical depth (AOD) and the instantaneous radiative forcing on climate were calculated online. Combined with model improvements, the results of the simulations are consistent with the observations of the various satellites. Slight deviations between the observations and model simulations were found for the large volcanic eruption of Pinatubo in 1991 and cases where simultaneous satellite observations were not unique or too sparse. Weak- and medium-strength volcanic eruptions captured in satellite data and the Smithsonian database typically inject about 10 to 50 kt SO2 directly into the upper troposphere/lower stratosphere (UTLS) region or the sulfur species are transported via convection and advection. Our results confirm that these relatively minor eruptions, which occur quite frequently, can nevertheless contribute to the stratospheric aerosol layer and are relevant for the Earth's radiation budget. These minor eruptions cause a total global instantaneous radiative forcing of the order of −0.1 W m−2 at the top of the atmosphere (TOA) compared to a background stratospheric aerosol forcing of about −0.04 W m−2. Medium-strength eruptions injecting about 400 kt SO2 into the stratosphere or accumulation of consecutive smaller eruptions can lead to a total instantaneous forcing of about −0.3 W m−2. We show that it is critical to include the contribution of the extratropical lowermost stratospheric aerosol in the forcing calculations.

Climate response to off-equatorial stratospheric sulfur injections in three Earth system models – Part 1: Experimental protocols and surface changes

Abstract. There is now substantial literature on climate model studies of equatorial or tropical stratospheric SO2 injections that aim to counteract the surface warming produced by rising concentrations of greenhouse gases. Here we present the results from the first systematic intercomparison of climate responses in three Earth system models wherein the injection of SO2 occurs at different latitudes in the lower stratosphere: CESM2-WACCM6, UKESM1.0 and GISS-E2.1-G. The first two use a modal aerosol microphysics scheme, while two versions of GISS-E2.1-G use a bulk aerosol (One-Moment Aerosol, OMA) and a two-moment (Multiconfiguration Aerosol TRacker of mIXing state, MATRIX) microphysics approach, respectively. Our aim in this work is to determine commonalities and differences between the climate model responses in terms of the distribution of the optically reflective sulfate aerosols produced from the oxidation of SO2 and in terms of the surface response to the resulting reduction in solar radiation. A focus on understanding the contribution of characteristics of models transport alongside their microphysical and chemical schemes, and on evaluating the resulting stratospheric responses in different models, is given in the companion paper (Bednarz et al., 2023). The goal of this exercise is not to evaluate these single-point injection simulations as stand-alone proposed strategies to counteract global warming; instead we determine sources and areas of agreement and uncertainty in the simulated responses and, ultimately, the possibility of designing a comprehensive intervention strategy capable of managing multiple simultaneous climate goals through the combination of different injection locations. We find large disagreements between GISS-E2.1-G and the CESM2-WACCM6 and UKESM1.0 models regarding the magnitude of cooling per unit of aerosol optical depth (AOD) produced, which varies from 4.7 K per unit of AOD in CESM2-WACCM6 to 16.7 K in the GISS-E2.1-G version with two-moment aerosol microphysics. By normalizing the results with the global mean response in each of the models and thus assuming that the amount of SO2 injected is a free parameter that can be managed independently, we highlight some commonalities in the overall distributions of the aerosols, in the inter-hemispheric surface temperature response and in shifts to the Intertropical Convergence Zone, as well as some areas of disagreement, such as the extent of the aerosol confinement in the equatorial region and the efficiency of the transport to polar latitudes. In conclusion, we demonstrate that it is possible to use these simulations to produce more comprehensive injection strategies in multiple climate models. However, large differences in the injection magnitudes can be expected, potentially increasing inter-model spreads in some stratospheric quantities (such as aerosol distribution) while reducing the spread in the surface response in terms of temperature and precipitation; furthermore, the selection of the injection locations may be dependent on the models' specific stratospheric transport.

Climate response to off-equatorial stratospheric sulfur injections in three Earth system models – Part 2: Stratospheric and free-tropospheric response

Abstract. The paper constitutes Part 2 of a study performing a first systematic inter-model comparison of the atmospheric responses to stratospheric aerosol injection (SAI) at various single latitudes in the tropics, as simulated by three state-of-the-art Earth system models – CESM2-WACCM6, UKESM1.0, and GISS-E2.1-G. Building on Part 1 (Visioni et al., 2023) we demonstrate the role of biases in the climatological circulation and specific aspects of the model microphysics in driving the inter-model differences in the simulated sulfate distributions. We then characterize the simulated changes in stratospheric and free-tropospheric temperatures, ozone, water vapor, and large-scale circulation, elucidating the role of the above aspects in the surface SAI responses discussed in Part 1. We show that the differences in the aerosol spatial distribution can be explained by the significantly faster shallow branches of the Brewer–Dobson circulation in CESM2, a relatively isolated tropical pipe and older tropical age of air in UKESM, and smaller aerosol sizes and relatively stronger horizontal mixing (thus very young stratospheric age of air) in the two GISS versions used. We also find a large spread in the magnitudes of the tropical lower-stratospheric warming amongst the models, driven by microphysical, chemical, and dynamical differences. These lead to large differences in stratospheric water vapor responses, with significant increases in stratospheric water vapor under SAI in CESM2 and GISS that were largely not reproduced in UKESM. For ozone, good agreement was found in the tropical stratosphere amongst the models with more complex microphysics, with lower stratospheric ozone changes consistent with the SAI-induced modulation of the large-scale circulation and the resulting changes in transport. In contrast, we find a large inter-model spread in the Antarctic ozone responses that can largely be explained by the differences in the simulated latitudinal distributions of aerosols as well as the degree of implementation of heterogeneous halogen chemistry on sulfate in the models. The use of GISS runs with bulk microphysics demonstrates the importance of more detailed treatment of aerosol processes, with contrastingly different stratospheric SAI responses to the models using the two-moment aerosol treatment; however, some problems in halogen chemistry in GISS are also identified that require further attention. Overall, our results contribute to an increased understanding of the underlying physical mechanisms as well as identifying and narrowing the uncertainty in model projections of climate impacts from SAI.

Volcanic stratospheric sulfur injections and aerosol optical depth during the Holocene (past 11 500 years) from a bipolar ice-core array

Abstract. The injection of sulfur into the stratosphere by volcanic eruptions is the dominant driver of natural climate variability on interannual to multidecadal timescales. Based on a set of continuous sulfate and sulfur records from a suite of ice cores from Greenland and Antarctica, the HolVol v.1.0 database includes estimates of the magnitudes and approximate source latitudes of major volcanic stratospheric sulfur injection (VSSI) events for the Holocene (from 9500 BCE or 11 500 years BP to 1900 CE), constituting an extension of the previous record by 7000 years. The database incorporates new-generation ice-core aerosol records with a sub-annual temporal resolution and a demonstrated sub-decadal dating accuracy and precision. By tightly aligning and stacking the ice-core records on the WD2014 chronology from Antarctica, we resolve long-standing inconsistencies in the dating of ancient volcanic eruptions that arise from biased (i.e., dated too old) ice-core chronologies over the Holocene for Greenland. We reconstruct a total of 850 volcanic eruptions with injections in excess of 1 teragram of sulfur (Tg S); of these eruptions, 329 (39 %) are located in the low latitudes with bipolar sulfate deposition, 426 (50 %) are located in the Northern Hemisphere extratropics (NHET) and 88 (10 %) are located in the Southern Hemisphere extratropics (SHET). The spatial distribution of the reconstructed eruption locations is in agreement with prior reconstructions for the past 2500 years. In total, these eruptions injected 7410 Tg S into the stratosphere: 70 % from tropical eruptions and 25 % from NH extratropical eruptions. A long-term latitudinally and monthly resolved stratospheric aerosol optical depth (SAOD) time series is reconstructed from the HolVol VSSI estimates, representing the first Holocene-scale reconstruction constrained by Greenland and Antarctica ice cores. These new long-term reconstructions of past VSSI and SAOD variability confirm evidence from regional volcanic eruption chronologies (e.g., from Iceland) in showing that the Early Holocene (9500–7000 BCE) experienced a higher number of volcanic eruptions (+16 %) and cumulative VSSI (+86 %) compared with the past 2500 years. This increase coincides with the rapid retreat of ice sheets during deglaciation, providing context for potential future increases in volcanic activity in regions under projected glacier melting in the 21st century. The reconstructed VSSI and SAOD data are available at https://doi.org/10.1594/PANGAEA.928646 (Sigl et al., 2021).

Volcanic stratospheric injections up to 160 Tg(S) yield a Eurasian winter warming indistinguishable from internal variability

Abstract. Early observational and modeling work suggested that low-latitude volcanic eruptions, comparable to the one of Pinatubo in 1991 or Krakatau in 1883, cause substantial surface warming over the northern continents at mid-latitudes in winter. The proposed mechanism consists of the formation of an anomalously strong Equator-to-pole temperature gradient in the stratosphere due to the presence of volcanic aerosols in the tropics, which are accompanied by an acceleration of the stratospheric polar vortex, which then shifts the Northern Annular Mode into a positive phase, resulting in warming surface temperatures over Eurasia. However, a large body of research in the past decade has shown that, for eruptions such as Pinatubo or Krakatau, no such warming is seen in simulations with more recent climate models which, in general, have much finer vertical and horizontal resolution than the early ones, and which have separated the forced response from the internal variability by using large ensembles of integrations. Since the proposed physical mechanism is sound, it is then possible that eruptions comparable to those of Pinatubo or Krakatau are simply too weak, but even larger ones might indeed be capable of causing Eurasian surface warming in winter. In this study, we explore this possibility using a state-of-the-art, stratosphere-resolving climate model, forced with prescribed aerosols from the Easy Volcanic Aerosol protocol. We consider eruptions with stratospheric sulfur injections of 5, 10, 20, 40, 80, and 160 Tg(S). With 20-member ensembles, we find that with injections of 20 Tg(S) or more – roughly twice the amplitude of the Pinatubo and Krakatau eruptions – our model simulates a winter surface warming over Eurasia, which is statistically significant with a t test given our 20-member ensembles. However, the forced volcanic signal on Eurasian winter surface temperatures is very small, barely exceeding the 1σ range of internal variability for the 160 Tg(S) injection case, and much smaller for smaller eruptions. Most importantly, the number of eruptions needed to establish statistical significance is considerably larger than the number of eruptions known to have occurred in the past 2000 years.

Geochemical ice-core constraints on the timing and climatic impact of Aniakchak II (1628BCE) and Thera (Minoan) volcanic eruptions.

Decades of research have focused on establishing the exact year and climatic impact of the Minoan eruption of Thera, Greece (c.1680 to 1500BCE). Ice cores offer key evidence to resolve this controversy, but attempts have been hampered by a lack of multivolcanic event synchronization between records. In this study, Antarctic and Greenland ice-core records are synchronized using a double bipolar sulfate marker, and calendar dates are assigned to each eruption revealed within the 'Thera period'. From this global-scale sequence of volcanic sulfate loading, we derive indications toward each eruption's latitude and potential to disrupt the climate system. Ultrafine sampling for sulfur isotopes and tephra conclusively demonstrate a colossal eruption of Alaska's Aniakchak II as the source of stratospheric sulfate in the now precisely dated1628 BCE ice layer. These findings end decades of speculation that Thera was responsible for the 1628BCE event, and place Aniakchak II (52 ± 17 Tg S) and an unknown volcano at 1654BCE (50 ± 13 Tg S) as two of the largest Northern Hemisphere sulfur injections in the last 4,000years. This opens possibilities to explore widespread climatic impacts for contemporary societies and, in pinpointing Aniakchak II, confirms that stratospheric sulfate can be globally distributed from eruptions outside the tropics. Dating options for Thera are reduced to a series of precisely dated, constrained stratospheric sulfur injection events at 1611BCE, 1561/1558/1555BCE, and c.1538BCE, which are all below 14 ± 5 Tg S, indicating a climatic forcing potential for Thera well below that of Tambora (1815CE).

La Plata Basin Hydroclimate Response to Solar Radiation Modification With Stratospheric Aerosol Injection

This study analyses the La Plata Basin (LPB) hydroclimate response to Solar Radiation Modification (SRM) with Stratospheric Aerosol Injection (SAI) in terms of changes in mean and extreme temperature, rainfall, and river flows simulations from the Geoengineering Large Ensemble (GLENS). The GLENS data used consists of three members simulations of a single model under the high anthropogenic emission scenario RCP8.5 with and without sulfur injection in the tropical stratosphere. The response of such an intervention is compared to a historical period (1980–2010) and to projections under the RCP8.5 scenario for two time slices: 2021–2050 and 2051–2080. The analysis of changes in extreme temperature and precipitation focuses on a subset of climate indices from the Expert Team of Climate Change Detection and Indices (ETCCDI). To determine the possible effects of SRM in the LPB water cycle, we use the distributed Variable Infiltration Capacity (VIC) hydrologic model in combination with daily extreme temperature and precipitation outputs from GLENS. Systematic errors in both fields were corrected by the application of a statistical bias correction method. Results show robust impacts on the water cycle of the LPB due to SRM implementation, particularly associated with increased precipitation over the northern part of the region and a general reduced warming compared to the RCP8.5 scenario. These variations would lead to regional-dependent responses in the river flows, mostly related to reductions in the severity of the extremely low flow conditions. Additionally, under the SRM scenario a reduction in extreme precipitation and a cooling effect on extreme temperatures could be expected over the LPB.

Stratospheric ozone response to sulfate aerosol and solar dimming climate interventions based on the G6 Geoengineering Model Intercomparison Project (GeoMIP) simulations

Abstract. This study assesses the impacts of stratospheric aerosol intervention (SAI) and solar dimming on stratospheric ozone based on the G6 Geoengineering Model Intercomparison Project (GeoMIP) experiments, called G6sulfur and G6solar. For G6sulfur, an enhanced stratospheric sulfate aerosol burden reflects some of the incoming solar radiation back into space to cool the surface climate, while for G6solar, the reduction in the global solar constant in the model achieves the same goal. Both experiments use the high emissions scenario of SSP5-8.5 as the baseline experiment and define surface temperature from the medium emission scenario of SSP2-4.5 as the target. In total, six Earth system models (ESMs) performed these experiments, and three out of the six models include interactive stratospheric chemistry. The increase in absorbing sulfate aerosols in the stratosphere results in a heating of the lower tropical stratospheric temperatures by between 5 to 13 K for the six different ESMs, leading to changes in stratospheric transport, water vapor, and other related changes. The increase in the aerosol burden also increases aerosol surface area density, which is important for heterogeneous chemical reactions. The resulting changes in the springtime Antarctic ozone between the G6sulfur and SSP5-8.5, based on the three models with interactive chemistry, include an initial reduction in total column ozone (TCO) of 10 DU (ranging between 0–30 DU for the three models) and up to 20 DU (between 10–40 DU) by the end of the century. The relatively small reduction in TCO for the multi-model mean in the first 2 decades results from variations in the required sulfur injections in the models and differences in the complexity of the chemistry schemes. In contrast, in the Northern Hemisphere (NH) high latitudes, no significant changes can be identified due to the large natural variability in the models, with little change in TCO by the end of the century. However, all three models with interactive chemistry consistently simulate an increase in TCO in the NH mid-latitudes up to 20 DU, compared to SSP5-8.5, in addition to the 20 DU increase resulting from increasing greenhouse gases between SSP2-4.5 and SSP5-8.5. In contrast to G6sulfur, G6solar does not significantly change stratospheric temperatures compared to the baseline simulation. Solar dimming results in little change in TCO compared to SSP5-8.5. Only in the tropics does G6solar result in an increase of TCO of up to 8 DU, compared to SSP2-4.5, which may counteract the projected reduction in SSP5-8.5. This work identifies differences in the response of SAI and solar dimming on ozone for three ESMs with interactive chemistry, which are partly due to the differences and shortcomings in the complexity of aerosol microphysics, chemistry, and the description of ozone photolysis. It also identifies that solar dimming, if viewed as an analog to SAI using a predominantly scattering aerosol, would succeed in reducing tropospheric and surface temperatures, but any stratospheric changes due to the high forcing greenhouse gas scenario, including the potential harmful increase in TCO beyond historical values, would prevail.

An interactive stratospheric aerosol model intercomparison of solar geoengineering by stratospheric injection of SO<sub>2</sub> or accumulation-mode sulfuric acid aerosols

Abstract. Studies of stratospheric solar geoengineering have tended to focus on modification of the sulfuric acid aerosol layer, and almost all climate model experiments that mechanistically increase the sulfuric acid aerosol burden assume injection of SO2. A key finding from these model studies is that the radiative forcing would increase sublinearly with increasing SO2 injection because most of the added sulfur increases the mass of existing particles, resulting in shorter aerosol residence times and aerosols that are above the optimal size for scattering. Injection of SO3 or H2SO4 from an aircraft in stratospheric flight is expected to produce particles predominantly in the accumulation-mode size range following microphysical processing within an expanding plume, and such injection may result in a smaller average stratospheric particle size, allowing a given injection of sulfur to produce more radiative forcing. We report the first multi-model intercomparison to evaluate this approach, which we label AM-H2SO4 injection. A coordinated multi-model experiment designed to represent this SO3- or H2SO4-driven geoengineering scenario was carried out with three interactive stratospheric aerosol microphysics models: the National Center for Atmospheric Research (NCAR) Community Earth System Model (CESM2) with the Whole Atmosphere Community Climate Model (WACCM) atmospheric configuration, the Max-Planck Institute's middle atmosphere version of ECHAM5 with the HAM microphysical module (MAECHAM5-HAM) and ETH's SOlar Climate Ozone Links with AER microphysics (SOCOL-AER) coordinated as a test-bed experiment within the Geoengineering Model Intercomparison Project (GeoMIP). The intercomparison explores how the injection of new accumulation-mode particles changes the large-scale particle size distribution and thus the overall radiative and dynamical response to stratospheric sulfur injection. Each model used the same injection scenarios testing AM-H2SO4 and SO2 injections at 5 and 25 Tg(S) yr−1 to test linearity and climate response sensitivity. All three models find that AM-H2SO4 injection increases the radiative efficacy, defined as the radiative forcing per unit of sulfur injected, relative to SO2 injection. Increased radiative efficacy means that when compared to the use of SO2 to produce the same radiative forcing, AM-H2SO4 emissions would reduce side effects of sulfuric acid aerosol geoengineering that are proportional to mass burden. The model studies were carried out with two different idealized geographical distributions of injection mass representing deployment scenarios with different objectives, one designed to force mainly the midlatitudes by injecting into two grid points at 30∘ N and 30∘ S, and the other designed to maximize aerosol residence time by injecting uniformly in the region between 30∘ S and 30∘ N. Analysis of aerosol size distributions in the perturbed stratosphere of the models shows that particle sizes evolve differently in response to concentrated versus dispersed injections depending on the form of the injected sulfur (SO2 gas or AM-H2SO4 particulate) and suggests that prior model results for concentrated injection of SO2 may be strongly dependent on model resolution. Differences among models arise from differences in aerosol formulation and differences in model dynamics, factors whose interplay cannot be easily untangled by this intercomparison.

Dependency of the impacts of geoengineering on the stratospheric sulfur injection strategy – Part 1: Intercomparison of modal and sectional aerosol modules

Abstract. Injecting sulfur dioxide into the stratosphere with the intent to create an artificial reflective aerosol layer is one of the most studied options for solar radiation management. Previous modelling studies have shown that stratospheric sulfur injections have the potential to compensate for the greenhouse-gas-induced warming at the global scale. However, there is significant diversity in the modelled radiative forcing from stratospheric aerosols depending on the model and on which strategy is used to inject sulfur into the stratosphere. Until now, it has not been clear how the evolution of the aerosols and their resulting radiative forcing depends on the aerosol microphysical scheme used – that is, if aerosols are represented by a modal or sectional distribution. Here, we have studied different spatio-temporal injection strategies with different injection magnitudes using the aerosol–climate model ECHAM-HAMMOZ with two aerosol microphysical modules: the sectional module SALSA (Sectional Aerosol module for Large Scale Applications) and the modal module M7. We found significant differences in the model responses depending on the aerosol microphysical module used. In a case where SO2 was injected continuously in the equatorial stratosphere, simulations with SALSA produced an 88 %–154 % higher all-sky net radiative forcing than simulations with M7 for injection rates from 1 to 100 Tg (S) yr−1. These large differences are identified to be caused by two main factors. First, the competition between nucleation and condensation: while injected sulfur tends to produce new particles at the expense of gaseous sulfuric acid condensing on pre-existing particles in the SALSA module, most of the gaseous sulfuric acid partitions to particles via condensation at the expense of new particle formation in the M7 module. Thus, the effective radii of stratospheric aerosols were 10 %–52 % larger in M7 than in SALSA, depending on the injection rate and strategy. Second, the treatment of the modal size distribution in M7 limits the growth of the accumulation mode which results in a local minimum in the aerosol number size distribution between the accumulation and coarse modes. This local minimum is in the size range where the scattering of solar radiation is most efficient. We also found that different spatial-temporal injection strategies have a significant impact on the magnitude and zonal distribution of radiative forcing. Based on simulations with various injection rates using SALSA, the most efficient studied injection strategy produced a 33 %–42 % radiative forcing compared with the least efficient strategy, whereas simulations with M7 showed an even larger difference of 48 %–116 %. Differences in zonal mean radiative forcing were even larger than that. We also show that a consequent stratospheric heating and its impact on the quasi-biennial oscillation depend on both the injection strategy and the aerosol microphysical model. Overall, these results highlight the crucial impact of aerosol microphysics on the physical properties of stratospheric aerosol which, in turn, causes significant uncertainties in estimating the climate impacts of stratospheric sulfur injections.

Sensitivity of Total Column Ozone to Stratospheric Sulfur Injection Strategies

AbstractWe explore the impact of different stratospheric sulfur injection strategies to counter greenhouse gas induced warming on total column ozone (TCO), including high and low altitude injections at four latitudes, equatorial injections, and using a configuration with higher vertical resolution, based on a state‐of‐the‐art Earth system model. The experiments maintain global surface temperatures at 2020 conditions, while following the unmitigated future scenario. Within the first 10 years of the injection, we find an abrupt deepening of the Antarctic ozone hole by 8%–20% and changes up to 5% for other regions and seasons. The ozone hole recovery is delayed by ∼25 to over 55 years, with the fastest recovery for low‐altitude injections and slowest for equatorial injections. Mid to high‐latitude TCO increases by 15% in Northern Hemisphere winter and spring between 2010–2019 and 2080–2089 due to both increasing greenhouse gases and increasing sulfur injections. Implications for ecosystems need to be investigated.

Atmosphere–ocean–aerosol–chemistry–climate model SOCOLv4.0: description and evaluation

Abstract. This paper features the new atmosphere–ocean–aerosol–chemistry–climate model, SOlar Climate Ozone Links (SOCOL) v4.0, and its validation. The new model was built by interactively coupling the Max Planck Institute Earth System Model version 1.2 (MPI-ESM1.2) (T63, L47) with the chemistry (99 species) and size-resolving (40 bins) sulfate aerosol microphysics modules from the aerosol–chemistry–climate model, SOCOL-AERv2. We evaluate its performance against reanalysis products and observations of atmospheric circulation, temperature, and trace gas distribution, with a focus on stratospheric processes. We show that SOCOLv4.0 captures the low- and midlatitude stratospheric ozone well in terms of the climatological state, variability and evolution. The model provides an accurate representation of climate change, showing a global surface warming trend consistent with observations as well as realistic cooling in the stratosphere caused by greenhouse gas emissions, although, as in previous model versions, a too-fast residual circulation and exaggerated mixing in the surf zone are still present. The stratospheric sulfur budget for moderate volcanic activity is well represented by the model, albeit with slightly underestimated aerosol lifetime after major eruptions. The presence of the interactive ocean and a successful representation of recent climate and ozone layer trends make SOCOLv4.0 ideal for studies devoted to future ozone evolution and effects of greenhouse gases and ozone-destroying substances, as well as the evaluation of potential solar geoengineering measures through sulfur injections. Potential further model improvements could be to increase the vertical resolution, which is expected to allow better meridional transport in the stratosphere, as well as to update the photolysis calculation module and budget of mesospheric odd nitrogen. In summary, this paper demonstrates that SOCOLv4.0 is well suited for applications related to the stratospheric ozone and sulfate aerosol evolution, including its participation in ongoing and future model intercomparison projects.