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While water and sulfuric acid droplets are the main component of stratospheric aerosols, measurements performed for about 30 years have shown that non-sulfate particles (NSPs) are also present. Such particles, released from the Earth mainly through volcanic eruptions, pollution or biomass burning, or coming from space, present a wide variety of compositions, sizes, and shapes. To better understand the origin of NSPs, we have performed measurements with the Light Optical Aerosol Counter (LOAC) during 151 flights under weather balloons in the 2013–2019 period reaching altitudes up to 35 km. Coupled with previous counting measurements conducted over the 2004–2011 period, the LOAC measurements indicate the presence of stratospheric layers of enhanced concentrations associated with NSPs, with a bimodal vertical repartition ranging between 17 and 30 km altitude. Such enhancements are not correlated with permanent meteor shower events. They may be linked to dynamical and photophoretic effects lifting and sustaining particles coming from the Earth. Besides, large particles, up to several tens of μm, were detected and present decreasing concentrations with increasing altitudes. All these particles can originate from Earth but also from meteoroid disintegrations and from the interplanetary dust cloud and comets.

Solar geoengineering by deliberate injection of sulfate aerosols in the stratosphere is one of the proposed options to counter anthropogenic climate warming. In this study, we focus on the effect of a specific microphysical property of sulfate aerosols in the stratosphere: hygroscopic growth—the tendency of particles to grow by accumulating water. We show that stratospheric sulfate aerosols, for a given mass of sulfates, cause more cooling when prescribed at the lower levels of the stratosphere because of hygroscopic growth. The larger relative humidity in the lower stratosphere causes an increase in the aerosol size through hygroscopic growth that leads to a larger scattering efficiency. In our study, hygroscopic growth provides an additional cooling of 23% (0.7 K) when 20 Mt‐SO4 of sulfate aerosols, an amount that approximately offsets the warming due to a doubling of CO2, are prescribed at 100 hPa. The hygroscopic effect becomes weaker at higher levels as relative humidity decreases with height. Hygroscopic growth also leads to secondary effects such as an increase in near‐infrared shortwave absorption by the aerosols that causes a decrease in high clouds and an increase in stratospheric water vapor. The altitude dependence of the effects of hygroscopic growth is opposite to that of sedimentation effects or the fast adjustment effects due to aerosol‐induced warming identified in a recent study. Plain Language Summary The injection of sulfate aerosols into the stratosphere is one of the proposed solar geoengineering methods to reduce anthropogenic warming. There are several uncertainties associated with the effects of stratospheric aerosol injection such as aerosol microphysics, transport, removal, and other physical and chemical changes of the aerosols. In this study, we have investigated the effects of a single source of uncertainty—the hygroscopic growth which depends on the ambient relative humidity in the stratosphere. Hygroscopic growth could lead to an increase in the size of the aerosols and consequently an increase in scattering efficiency. As the relative humidity is larger in the lower stratosphere, we find that the cooling efficiency of a fixed mass of sulfates is larger when they are prescribed in the lower levels of the stratosphere. This effect of hygroscopic growth can be substantial: for 20 Mt‐SO4 that offsets the warming from a doubling of CO2, we find an additional cooling of about 20%. Our results indicate the need for an accurate parametrization of aerosol microphysical and radiative processes in climate models for an improved understanding of the effects of stratospheric aerosol injection. Key Points The effects of hygroscopic growth of sulfate aerosols in stratospheric aerosol geoengineering are investigated A specified mass of sulfates is more efficient in cooling the climate when they reside in the lower stratosphere due to hygroscopic growth Hygroscopic growth can provide ~20% additional cooling when sulfates are used to offset warming from a doubling of CO2

In this paper, we focus on stratospheric sulfate injection as a geoengineering scheme, and provide a combined scientific and ethical analysis of climate response tests, which are a subset of outdoor tests that would seek to impose detectable and attributable changes to climate variables on global or regional scales. We assess the current state of scientific understanding on the plausibility and scalability of climate response tests. Then, we delineate a minimal baseline against which to consider whether certain climate response tests would be relevant for a deployment scenario. Our analysis shows that some climate response tests, such as those attempting to detect changes in regional climate impacts, may not be deployable in time periods relevant to realistic geoengineering scenarios. This might pose significant challenges for justifying stratospheric sulfate aerosol injection deployment overall. We then survey some of the major ethical challenges that proposed climate response tests face. We consider what levels of confidence would be required to ethically justify approving a proposed test; whether the consequences of tests are subject to similar questions of justice, compensation, and informed consent as full‐scale deployment; and whether questions of intent and hubris are morally relevant for climate response tests. We suggest further research into laboratory‐based work and modeling may help to narrow the scientific uncertainties related to climate response tests, and help inform future ethical debate. However, even if such work is pursued, the ethical issues raised by proposed climate response tests are significant and manifold. Key Points Climate response tests aimed at detecting changes in regional climate impacts may not be achievable in time scales relevant for deployment Other possible climate response tests face difficult ethical questions around uncertainty, justice, compensation, consent, intent, and hubris Further research may help to narrow the scientific uncertainties related to climate response tests, and help inform future ethical debate

We present here results from the Geoengineering Model Intercomparison Project (GeoMIP) simulations for the experiments G6sulfur and G6solar for six Earth system models participating in the Climate Model Intercomparison Project (CMIP) Phase 6. The aim of the experiments is to reduce the warming that results from a high-tier emission scenario (Shared Socioeconomic Pathways SSP5-8.5) to that resulting from a medium-tier emission scenario (SSP2-4.5). These simulations aim to analyze the response of climate models to a reduction in incoming surface radiation as a means to reduce global surface temperatures, and they do so either by simulating a stratospheric sulfate aerosol layer or, in a more idealized way, through a uniform reduction in the solar constant in the model. We find that over the final two decades of this century there are considerable inter-model spreads in the needed injection amounts of sulfate (29 ± 9 Tg-SO2/yr between 2081 and 2100), in the latitudinal distribution of the aerosol cloud and in the stratospheric temperature changes resulting from the added aerosol layer. Even in the simpler G6solar experiment, there is a spread in the needed solar dimming to achieve the same global temperature target (1.91 ± 0.44 %). The analyzed models already show significant differences in the response to the increasing CO2 concentrations for global mean temperatures and global mean precipitation (2.05 K ± 0.42 K and 2.28 ± 0.80 %, respectively, for SSP5-8.5 minus SSP2-4.5 averaged over 2081–2100). With aerosol injection, the differences in how the aerosols spread further change some of the underlying uncertainties, such as the global mean precipitation response (−3.79 ± 0.76 % for G6sulfur compared to −2.07 ± 0.40 % for G6solar against SSP2-4.5 between 2081 and 2100). These differences in the behavior of the aerosols also result in a larger uncertainty in the regional surface temperature response among models in the case of the G6sulfur simulations, suggesting the need to devise various, more specific experiments to single out and resolve particular sources of uncertainty. The spread in the modeled response suggests that a degree of caution is necessary when using these results for assessing specific impacts of geoengineering in various aspects of the Earth system. However, all models agree that compared to a scenario with unmitigated warming, stratospheric aerosol geoengineering has the potential to both globally and locally reduce the increase in surface temperatures.

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.

It has been suggested that increased stratospheric sulfate aerosol loadings following large, low latitude volcanic eruptions can lead to wintertime warming over Eurasia through dynamical stratosphere–troposphere coupling. We here investigate the proposed connection in the context of hypothetical future stratospheric sulfate geoengineering in the Geoengineering Large Ensemble simulations. In those geoengineering simulations, we find that stratospheric circulation anomalies that resemble the positive phase of the Northern Annular Mode in winter are a distinguishing climate response which is absent when increasing greenhouse gases alone are prescribed. This stratospheric dynamical response projects onto the positive phase of the North Atlantic Oscillation, leading to associated side effects of this climate intervention strategy, such as continental Eurasian warming and precipitation changes. Seasonality is a key signature of the dynamically driven surface response. We find an opposite response of the North Atlantic Oscillation in summer, when no dynamical role of the stratosphere is expected. The robustness of the wintertime forced response stands in contrast to previously proposed volcanic responses.

Solar radiation management is increasingly considered to be an option for managing global temperatures 1 , 2 , yet the economic effects of ameliorating climatic changes by scattering sunlight back to space remain largely unknown 3 . Although solar radiation management may increase crop yields by reducing heat stress 4 , the effects of concomitant changes in available sunlight have never been empirically estimated. Here we use the volcanic eruptions that inspired modern solar radiation management proposals as natural experiments to provide the first estimates, to our knowledge, of how the stratospheric sulfate aerosols created by the eruptions of El Chichón and Mount Pinatubo altered the quantity and quality of global sunlight, and how these changes in sunlight affected global crop yields. We find that the sunlight-mediated effect of stratospheric sulfate aerosols on yields is negative for both C4 (maize) and C3 (soy, rice and wheat) crops. Applying our yield model to a solar radiation management scenario based on stratospheric sulfate aerosols, we find that projected mid-twenty-first century damages due to scattering sunlight caused by solar radiation management are roughly equal in magnitude to benefits from cooling. This suggests that solar radiation management—if deployed using stratospheric sulfate aerosols similar to those emitted by the volcanic eruptions it seeks to mimic—would, on net, attenuate little of the global agricultural damage from climate change. Our approach could be extended to study the effects of solar radiation management on other global systems, such as human health or ecosystem function. Analysis of the El Chichón and Mount Pinatubo volcanic eruptions suggests that solar radiation management strategies using stratospheric sulfate aerosols would do little to counterbalance the effects of climate change on global crop yields.

Stratospheric sulfate aerosols from tropical volcanic eruptions alter surface air temperatures. Fundamentally, this is due to two different properties of the aerosols: Their ability to reflect incoming solar shortwave radiation, and their ability to absorb terrestrial longwave radiation. However, the relatedness and dynamical consequences of the two properties are unclear. Here we show that in a state‐of‐the art climate model the two properties have independent and fundamentally different impacts on zonal asymmetries of Northern Hemisphere extra‐tropical winter temperatures: The shortwave properties induce a tropospheric Rossby wave train apparently connected to changes in tropical convection. The longwave properties imprint a wavenumber 1‐like signal on surface temperatures related to altered stratospheric winds. The independence of these responses provides a useful starting point for analyzing the extra‐tropical temperature response to volcanic eruptions in both observations and models.

In situ carbonyl sulfide (OCS) measurements from the Stratospheric Aerosol processes, Budget and Radiative Effects (SABRE) 2023 airborne campaign are used to evaluate the sulfate budget in the Arctic stratosphere during boreal winter. The strong correspondence between these measurements and remote retrievals from the Atmospheric Chemistry Experiment–Fourier Transform Spectrometer provide robust validation of the satellite's capability to monitor stratospheric OCS globally. We demonstrate how trends in the tropical tropopause layer and National Oceanic and Atmospheric Administration OCS surface data reveal a post‐2016 ∼8% global decline in OCS abundance, which is absent from many global climate models. New simulations with a revised planetary boundary layer OCS abundance show improved agreement with remote retrievals and in situ data across multiple stratospheric layers, but remaining model biases highlight the need for additional in situ OCS observations. The revised representation reduces the stratospheric sulfate burden, resulting in an increased shortwave solar flux at the tropical tropopause by as much as 0.3 Wm−2 locally, with implications for stratospheric circulation, radiative forcing, and climate feedbacks.

The enhancement of the stratospheric sulfate aerosol layer has been proposed as a method of geoengineering to abate global warming. Previous modelling studies found that stratospheric aerosol geoengineering (SAG) could effectively compensate for the warming by greenhouse gases on the global scale, but also that the achievable cooling effect per sulfur mass unit, i.e. the forcing efficiency, decreases with increasing injection rate. In this study we use the atmospheric general circulation model LMDZ with the sectional aerosol module S3A to determine how the forcing efficiency depends on the injected amount of SO2, the injection height, and the spatio-temporal pattern of injection. We find that the forcing efficiency may decrease more drastically for larger SO2 injections than previously estimated. As a result, the net instantaneous radiative forcing does not exceed the limit of –2 Wm-2 for continuous equatorial SO2 injections and it decreases (in absolute value) for injection rates larger than 20 TgSyr-1. In contrast to other studies, the net radiative forcing in our experiments is fairly constant with injection height (in a range 17 to 23 km) for a given amount of SO2 injected. Also, spreading the SO2 injections between 30∘ S and 30∘ N or injecting only seasonally from varying latitudes does not result in a significantly larger (i.e. more negative) radiative forcing. Other key characteristics of our simulations include a consequent stratospheric heating, caused by the absorption of solar and infrared radiation by the aerosol, and changes in stratospheric dynamics, with a collapse of the quasi-biennial oscillation at larger injection rates, which has impacts on the resulting spatial aerosol distribution, size, and optical properties. But it has to be noted that the complexity and uncertainty of stratospheric processes cause considerable disagreement among different modelling studies of stratospheric aerosol geoengineering. This may be addressed through detailed model intercomparison activities, as observations to constrain the simulations of stratospheric aerosol geoengineering are not available and analogues (such as volcanic eruptions) are imperfect.