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Recent studies have suggested that injection of solid particles such as alumina and calcite particles for stratospheric aerosol injection (SAI) instead of sulfur-based injections could reduce some of the adverse side effects of SAI such as ozone depletion and stratospheric heating. Here, we present a version of the global aerosol–chemistry–climate model SOCOL-AERv2 and the Earth system model (ESM) SOCOLv4 which incorporate a solid-particle microphysics scheme for assessment of SAI of solid particles. Microphysical interactions of the solid particle with the stratospheric sulfur cycle were interactively coupled to the heterogeneous chemistry scheme and the radiative transfer code (RTC) for the first time within an ESM. Therefore, the model allows simulation of heterogeneous chemistry at the particle surface as well as feedbacks between microphysics, chemistry, radiation and climate. We show that sulfur-based SAI results in a doubling of the stratospheric aerosol burden compared to the same mass injection rate of calcite and alumina particles with a radius of 240 nm. Most of the sulfuric acid aerosol mass resulting from SO2 injection does not need to be lifted to the stratosphere but is formed after in situ oxidation and subsequent water uptake in the stratosphere. Therefore, to achieve the same radiative forcing, larger injection rates are needed for calcite and alumina particle injection than for sulfur-based SAI. The stratospheric sulfur cycle would be significantly perturbed, with a reduction in stratospheric sulfuric acid burden by 53 %, when injecting 5 Mtyr-1 (megatons per year) of alumina or calcite particles of 240 nm radius. We show that alumina particles will acquire a sulfuric acid coating equivalent to about 10 nm thickness if the sulfuric acid is equally distributed over the whole available particle surface area in the lower stratosphere. However, due to the steep contact angle of sulfuric acid on alumina particles, the sulfuric acid coating would likely not cover the entire alumina surface, which would result in available surface for heterogeneous reactions other than the ones on sulfuric acid. When applying realistic uptake coefficients of 1.0, 10-5 and 10-4 for H2SO4 , HCl and HNO3 , respectively, the same scenario with injections of calcite particles results in 94 % of the particle mass remaining in the form of CaCO3. This likely keeps the optical properties of the calcite particles intact but could significantly alter the heterogeneous reactions occurring on the particle surfaces. The major process uncertainties of solid-particle SAI are (1) the solid-particle microphysics in the injection plume and degree of agglomeration of solid particles on the sub-ESM grid scale, (2) the scattering properties of the resulting agglomerates, (3) heterogeneous chemistry on the particle surface, and (4) aerosol–cloud interactions. These uncertainties can only be addressed with extensive, coordinated experimental and modelling research efforts. The model presented in this work offers a useful tool for sensitivity studies and incorporating new experimental results on SAI of solid particles. [ABSTRACT FROM AUTHOR]

The rate of rocket launches is accelerating, driven by the rapid global development of the space industry. Rocket launches emit gases and particulates into the stratosphere, where they impact the ozone layer via radiative and chemical processes. We create a three‐dimensional per‐vehicle inventory of stratospheric emissions, accounting for flight profiles and all major fuel types in active use (solid, kerosene, cryogenic and hypergolic). In 2019, stratospheric (15–50 km) rocket launch emissions were 5.82 Gg CO2 ${\mathrm{C}\mathrm{O}}_{2}$, 6.38 Gg H2 ${\mathrm{H}}_{2}$O, 0.28 Gg black carbon, 0.22 Gg nitrogen oxides, 0.50 Gg reactive chlorine and 0.91 Gg particulate alumina. The geographic locations of launch sites are preserved in the inventory, which covers all active launch sites in 2019. We also report the emissions data from contemporary vehicles that were not launched in 2019, so that users have freedom to construct their own launch activity scenarios. A subset of the inventory—stratospheric emissions for successful launches in 2019—is freely available and formatted for direct use in global chemistry‐climate or Earth system models. Plain Language Summary: Many governments and companies have expressed bold ambitions to grow their presence in space. However, rocket launches throw out a stream of air pollutants from their burnt fuel as they pass through the stratosphere, which is where the protective ozone layer resides. Currently, launch operators do not have to measure the impacts of their activities on the ozone layer. We gather together all the publicly available information on rocket launches in 2019, from 18 active spaceports worldwide, and make some careful assumptions to convert each rocket's fuel to its burnt fuel products left in the atmosphere. We encourage modeling groups to use our inventory for studies on how rocket launches may impact the ozone layer. Key Points: We compile a comprehensive emissions inventory of all rocket launches in 2019 at 18 active spaceportsIt itemizes chemically and radiatively active species that are produced by the main rocket fuels (kerosene, cryogenic, solid and hypergolic)We discuss the inventory's uncertainties and its usage in global models to study the impacts of rocket launches on the ozone layer [ABSTRACT FROM AUTHOR]

Solar particle events (SPEs) are short-lived bursts of high-energy particles from the solar atmosphere and are widely recognized as posing significant economic risks to modern society. Most SPEs are relatively weak and have minor impacts on the Earth's environment, but historic records contain much stronger SPEs which have the potential to alter atmospheric chemistry, impacting climate and biological life. The impacts of such strong SPEs would be far more severe when the Earth's protective geomagnetic field is weak, such as during past geomagnetic excursions or reversals. Here, we model the impacts of an extreme SPE under different geomagnetic field strengths, focusing on changes in atmospheric chemistry and surface radiation using the atmosphere-ocean-chemistry-climate model SOCOL3-MPIOM and the radiation transfer model LibRadtran. Under current geomagnetic conditions, an extreme SPE would increase NOx concentrations in the polar stratosphere and mesosphere, causing reductions in extratropical stratospheric ozone lasting for about a year. In contrast, with no geomagnetic field, there would be a substantial increase in NOx throughout the entire atmosphere, resulting in severe stratospheric ozone depletion for several years. The resulting ground-level ultraviolet (UV) radiation would remain elevated for up to 6 y, leading to increases in UV index up to 20 to 25% and solar-induced DNA damage rates by 40 to 50%. The potential evolutionary impacts of past extreme SPEs remain an important question, while the risks they pose to human health in modern conditions continue to be underestimated. [ABSTRACT FROM AUTHOR]

Solar radiation modification by a sustained deliberate source of SO2 into the stratosphere (strat-SRM) has been proposed as an option for climate intervention. Global interactive aerosol–chemistry–climate models are often used to investigate the potential cooling efficiencies and associated side effects of hypothesized strat-SRM scenarios. A recent model intercomparison study for composition–climate models with interactive stratospheric aerosol suggests that the modeled climate response to a particular assumed injection strategy depends on the type of aerosol microphysical scheme used (e.g., modal or sectional representation) alongside host model resolution and transport. Compared to short-duration volcanic SO2 emissions, the continuous SO2 injections in strat-SRM scenarios may pose a greater challenge to the numerical implementation of microphysical processes such as nucleation, condensation, and coagulation. This study explores how changing the time steps and sequencing of microphysical processes in the sectional aerosol–chemistry–climate model SOCOL-AERv2 (40 mass bins) affects model-predicted climate and ozone layer impacts considering strat-SRM by SO2 injections of 5 and 25 Tg(S) yr −1 at 20 km altitude between 30° S and 30° N. The model experiments consider the year 2040 to be the boundary conditions for ozone-depleting substances and greenhouse gases (GHGs). We focus on the length of the microphysical time step and the call sequence of nucleation and condensation, the two competing sink processes for gaseous H2SO4. Under stratospheric background conditions, we find no effect of the microphysical setup on the simulated aerosol properties. However, at the high sulfur loadings reached in the scenarios injecting 25 Tg(S) yr −1 of SO2 with a default microphysical time step of 6 min, changing the call sequence from the default "condensation first" to "nucleation first" leads to a massive increase in the number densities of particles in the nucleation mode (R<0.01 µm) and a small decrease in coarse-mode particles (R>1 µm). As expected, the influence of the call sequence becomes negligible when the microphysical time step is reduced to a few seconds, with the model solutions converging to a size distribution with a pronounced nucleation mode. While the main features and spatial patterns of climate forcing by SO 2 injections are not strongly affected by the microphysical configuration, the absolute numbers vary considerably. For the extreme injection with 25 Tg(S) yr −1 , the simulated net global radiative forcing ranges from - 2.3 to - 5.3 Wm-2 , depending on the microphysical configuration. Nucleation first shifts the size distribution towards radii better suited for solar scattering (0.3 µm

We apply the Entire Atmosphere GLobal (EAGLE) model to investigate the upper atmosphere response to the January 2009 sudden stratospheric warming (SSW) event. The model successfully reproduces neutral temperature and total electron content (TEC) observations. Using both model and observational data, we identify a cooling in the tropical lower thermosphere caused by the SSW. This cooling affects the zonal electric field close to the equator, leading to an enhanced vertical plasma drift. We demonstrate that along with a SSW-related wind disturbance, which is the main source to form a dynamo electric field in the ionosphere, perturbations of the ionospheric conductivity also make a significant contribution to the formation of the electric field response to SSW. The post-sunset TEC enhancement and pre-sunrise electron content reduction are revealed as a response to the 2009 SSW. We show that at post-sunset hours the SSW affects low-latitude TEC via a disturbance of the meridional electric field. We also show that the phase change of the semidiurnal migrating solar tide (SW2) in the neutral wind caused by the 2009 SSW at the altitude of the dynamo electric field generation has a crucial importance for the SW2 phase change in the zonal electric field. Such changes lead to the appearance of anomalous diurnal variability of the equatorial electromagnetic plasma drift and subsequent low-latitudinal TEC disturbances in agreement with available observations. Plain Language Summary – Entire Atmosphere GLobal model (EAGLE) interactively calculates the troposphere, stratosphere, mesosphere, thermosphere, and plasmasphere–ionosphere system states and their response to various natural and anthropogenic forcing. In this paper, we study the upper atmosphere response to the major sudden stratospheric warming that occurred in January 2009. Our results agree well with the observed evolution of the neutral temperature in the upper atmosphere and with low-latitude ionospheric disturbances over America. For the first time, we identify an SSW-related cooling in the tropical lower thermosphere that, in turn, could provide additional information for understanding the mechanisms for the generation of electric field disturbances observed at low latitudes. We show that the SSW-related vertical electromagnetic drift due to electric field disturbances is a key mechanism for interpretation of an observed anomalous diurnal development of the equatorial ionization anomaly during the 2009 SSW event. We demonstrate that the link between thermospheric winds and the ionospheric dynamo electric field during the SSW is attained through the modulation of the semidiurnal migrating solar tide.

Stratospheric ozone is expected to recover by the mid-century due to the success of the Montreal Protocol in regulating the emission of ozone-depleting substances (ODSs). In the Arctic, ozone abundances are projected to surpass historical levels due to the combined effect of decreasing ODSs and elevated greenhouse gases (GHGs). While long-term changes in stratospheric ozone have been shown to be a major driver of future surface climate in the Southern Hemisphere during summertime, the dynamical and climatic impacts of elevated ozone levels in the Arctic have not been investigated. In this study, we use two chemistry climate models (the SOlar Climate Ozone Links – Max Planck Ocean Model (SOCOL-MPIOM) and the Community Earth System Model – Whole Atmosphere Community Climate Model (CESM-WACCM)) to assess the climatic impacts of future changes in Arctic ozone on stratospheric dynamics and surface climate in the Northern Hemisphere (NH) during the 21st century. Under the high-emission scenario (RCP8.5) examined in this work, Arctic ozone returns to pre-industrial levels by the middle of the century. Thereby, the increase in Arctic ozone in this scenario warms the lower Arctic stratosphere; reduces the strength of the polar vortex, advancing its breakdown; and weakens the Brewer–Dobson circulation. The ozone-induced changes in springtime generally oppose the effects of GHGs on the polar vortex. In the troposphere, future changes in Arctic ozone induce a negative phase of the Arctic Oscillation, pushing the jet equatorward over the North Atlantic. These impacts of future ozone changes on NH surface climate are smaller than the effects of GHGs, but they are remarkably robust among the two models employed in this study, canceling out a portion of the GHG effects (up to 20 % over the Arctic). In the stratosphere, Arctic ozone changes cancel out a much larger fraction of the GHG-induced signal (up to 50 %–100 %), resulting in no overall change in the projected springtime stratospheric northern annular mode and a reduction in the GHG-induced delay of vortex breakdown of around 15 d. Taken together, our results indicate that future changes in Arctic ozone actively shape the projected changes in the stratospheric circulation and their coupling to the troposphere, thereby playing an important and previously unrecognized role as a driver of the large-scale atmospheric circulation response to climate change. [ABSTRACT FROM AUTHOR]

Solar radiation management as a sustained deliberate source of SO2 into the stratosphere (strat-SRM) has been proposed as an option for climate intervention. Global interactive aerosol-chemistry-climate models are often used to investigate the potential cooling efficiencies and side effects of hypothesised strat-SRM scenarios. A recent strat-SRM model intercompar-ison study for composition-climate models with interactive stratospheric aerosol suggests that the modelled climate response 5 to a particular assumed injection strategy, depends on the type of aerosol microphysical scheme used (e.g., modal or sectional representation), alongside also host model resolution and transport. Compared to short-duration volcanic SO2 emission, the continuous SO2 injections in strat-SRM scenarios may pose a greater challenge to the numerical implementation of of microphysical processes such as nucleation, condensation, and coagulation. This study explores how changing the timesteps and sequencing of microphysical processes in the sectional aerosol-chemistry-climate model SOCOL-AERv2 (40 size bins) 10 affect model predicted climate and ozone layer impacts considering strat-SRM SO2 injections of of 5 and 25 Tg(S) yr-1 at 20 km altitude between 30°S and 30°N. The model experiments consider year 2040 boundary conditions for ozone depleting substances and green house gases. We focus on the length of the microphysical timestep and the call sequence of nucleation and condensation, the two competing sink processes for gaseous H2SO4. Under stratospheric background conditions, we find no effect of the microphysical setup on the simulated aerosol properties. However, at the high sulfur loadings reached in the 15 scenarios injecting 25 Mt/yr of sulfur with a default microphysical timesetp of 6 min, changing the call sequence from the default "condensation first" to "nucleation first" leads to a massive increase in the number densities of particles in the nucle-ation mode (R < 0.01 µm) and a small decrease in coarse mode particles (R > 1 µm). As expected, the influence of the call sequence becomes negligible when the microphysical timestep is reduced to a few seconds, with the model solutions converging to a size distribution with a pronounced nucleation mode. While the main features and spatial patterns of climate forcing 20 by SO2 injections are not strongly affected by the microphysical configuration, the absolute numbers vary considerably. For the extreme injection with 25 Tg(S) yr-1, the simulated net global radiative forcing ranges from -2.3 W m-2 to -5.3 W m-2, depending on the microphysical configuration. "Nucleation first" shifts the size distribution towards radii better suited for solar scattering (0.3 µm < R < 0.4 µm), enhancing the intervention efficiency. The size-distribution shift however generates more ultra-fine aerosol particles, increasing the surface area density, resulting in 10 DU less ozone (about 3% of total column) in 25 the northern midlatitudes and 20 DU less ozone (6%) over the polar caps, compared to the "condensation first" approach. Our results suggest that a reasonably short microphysical time step of 2 minutes or less must be applied to accurately capture the magnitude of the H2SO2 supersaturation resulting from SO2 injection scenarios or volcanic eruptions. Taken together these results underscore how structural aspects of model representation of aerosol microphysical processes become important under conditions of elevated stratospheric sulfur in determining atmospheric chemistry and climate impacts. [ABSTRACT FROM AUTHOR]

Stratospheric ozone is expected to recover by mid-century due to the success of the Montreal Protocol in regulating the emission of ozone-depleting substances (ODSs). In the Arctic, ozone abundances are projected to surpass historical levels due to the combined effect of decreasing ODSs and elevated greenhouse gases (GHGs). While ozone recovery has been shown to be a major driver of future surface climate in the Southern Hemisphere during summertime, the dynamical and climatic impacts of elevated ozone levels in the Arctic have not been investigated. In this study, we use two chemistry climate models (SOCOL-MPIOM and CESM-WACCM) to assess the climatic impacts of Arctic ozone recovery on stratospheric dynamics and surface climate in the Northern Hemisphere (NH) during the 21st century. Under the high-emission scenario (RCP8.5) examined in this work, Arctic ozone returns to pre-industrial levels by the middle of the century. Thereby, it warms the lower Arctic stratosphere, reduces the strength of the polar vortex, advancing its breakdown, and weakening the Brewer-Dobson circulation. In the troposphere, Arctic ozone recovery induces a negative phase of the Arctic Oscillation, pushing the jet equatorward over the Atlantic. These impacts of ozone recovery in the NH are smaller than the effects of GHGs, but they are remarkably robust among the two models employed in this study, cancelling out some of the GHG effects. Taken together, our results indicate that Arctic ozone recovery actively shapes the projected changes in the stratospheric circulation and their coupling to the troposphere, thereby playing an important and previously unrecognized role as driver of the large-scale atmospheric circulation response to climate change [ABSTRACT FROM AUTHOR]

It is now recognized and confirmed that the ozone layer shields the biosphere from dangerous solar UV radiation and is also important for the global atmosphere and climate. The observed massive ozone depletion forced the introduction of limitations on the production of halogen-containing ozone-depleting substances (hODSs) by the Montreal Protocol and its amendments and adjustments (MPA). Previous research has demonstrated the success of the Montreal Protocol and increased public awareness of its necessity. In this study, we evaluate the benefits of the Montreal Protocol on climate and ozone evolution using the Earth system model (ESM) SOCOLv4.0 (modeling tools for studies of SOlar Climate Ozone Links) which includes dynamic modules for the ocean, sea ice, interactive ozone, and stratospheric aerosol. Here, we analyze the results of the numerical experiments performed with and without limitations on the ozone-depleting substance (ODS) emissions. In the experiments, we have used CMIP6 (Coupled Model Intercomparison Project) SSP2-4.5 and SSP5-8.5 (Shared Socioeconomic Pathway) scenarios for future forcing behavior. We confirm previous results regarding catastrophic ozone layer depletion and substantial climate warming in the case without MPA limitations. We show that the climate effects of MPA consist of additional global-mean warming by up to 2.5 K in 2100 caused by the direct radiative effect of the hODSs, which is comparable to large climate warming obtained with the SSP5-8.5 scenario. For the first time, we reveal the dramatic effects of MPA on chemical species and cloud cover. The response of surface temperature, precipitation, and sea-ice fields was demonstrated for the first time with the model that has interactive tropospheric and stratospheric chemistry. We have found some differences in the climate response compared to the model with prescribed ozone, which should be further addressed. Our research updates and complements previous modeling studies on the quantifying of MPA benefits for the terrestrial atmosphere and climate. [ABSTRACT FROM AUTHOR]

This study evaluates the future evolution of atmospheric ozone simulated with the Earth system model (ESM) SOCOLv4. Simulations have been performed based on two potential shared socioeconomic pathways (SSPs): the middle-of-the-road (SSP2-4.5) and fossil-fueled (SSP5-8.5) scenarios. The future changes in ozone, as well as in chemical drivers (NO x and CO) and temperature, were estimated between 2015 and 2099 and for several intermediate subperiods (i.e., 2015–2039, 2040–2069, and 2070–2099) via dynamic linear modeling. In both scenarios, the model projects a decline in tropospheric ozone in the future that starts in the 2030s in SSP2-4.5 and after the 2060s in SSP5-8.5 due to a decrease in concentrations of NO x and CO. The results also suggest a very likely ozone increase in the mesosphere and the upper and middle stratosphere, as well as in the lower stratosphere at high latitudes. Under SSP5-8.5, the ozone increase in the stratosphere is higher because of stronger cooling (>1 K per decade) induced by greenhouse gases (GHGs), which slows the catalytic ozone destruction cycles. In contrast, in the tropical lower stratosphere, ozone concentrations decrease in both experiments and increase over the middle and high latitudes of both hemispheres due to the speeding up of the Brewer–Dobson circulation, which is stronger in SSP5-8.5. No evidence was found of a decline in ozone levels in the lower stratosphere at mid-latitudes. In both future scenarios, the total column ozone is expected to be distinctly higher than present in middle to high latitudes and might be lower in the tropics, which causes a decrease in the mid-latitudes and an increase in the tropics in the surface level of ultraviolet radiation. The results of SOCOLv4 suggest that the stratospheric-ozone evolution throughout the 21st century is strongly governed not only by a decline in halogen concentration but also by future GHG forcing. In addition, the tropospheric-ozone column changes, which are mainly due to the changes in anthropogenic emissions of ozone precursors, also have a strong impact on the total column. Therefore, even though the anthropogenic halogen-loading problem has been brought under control to date, the sign of future ozone column changes, globally and regionally, is still unclear and largely depends on diverse future human activities. The results of this work are, thus, relevant for developing future strategies for socioeconomic pathways. [ABSTRACT FROM AUTHOR]

The Montreal Protocol and its amendments (MPA) have been a huge success in preserving the stratospheric ozone layer from being destroyed by unabated chlorofluorocarbons (CFCs) emissions. The phase out of CFCs has not only prevented serious impacts on our health and climate, but also avoided strong alterations of atmospheric circulation patterns. With the Earth System Model SOCOLv4, we study the dynamical and climatic impacts of a scenario with unabated CFC emissions by 2100, disentangling radiative and chemical (ozone-mediated) effects of CFCs. In the stratosphere, chemical effects of CFCs (i.e. the resulting ozone loss) are the main drivers of circulation changes, weakening wintertime polar vortices and speeding up the Brewer-Dobson circulation. These dynamical impacts during wintertime are due to low-latitude ozone depletion and resulting reduction of the equator-to-pole temperature gradient. In Southern Hemisphere (SH) summer, the vortex strengthens, similar due to the effects of the Antarctic ozone hole over the second half of the 20th century. Furthermore, the winter and spring vortex variability increases in the SH, whereas it decreases in summer and fall. This seasonal variation of wind speed in the stratosphere has regional implications on the tropospheric circulation modes. We find coherent changes in the troposphere, such as negative Southern Annular mode (SAM) and North Atlantic Oscillation (NAO) during seasons with a weaker vortex (winter and spring); the opposite occurs during seasons with stronger westerlies in the stratosphere (summer). In the troposphere, radiative heating by CFCs prevails throughout the year, shifting the SAM into a positive phase and canceling out the ozone induced effects on the NAO. Furthermore, global warming is amplified by 1.9 K with regionally up to 12 K increase over Eastern Canada andWestern Arctic. Our study sheds light into the adverse effects of a non-adherence to the MPA on the global atmospheric circulation, uncovering the roles of the underlying physical mechanisms. In so doing, our study emphasizes the importance of the MPA for Earth's climate, to avoid regional amplifications of negative climate impacts. [ABSTRACT FROM AUTHOR]