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Secondary organic aerosol (SOA) constitutes an important component of atmospheric particulate matter, with a substantial influence on air quality, human health and the global climate. The volatility basis set (VBS) framework has provided a valuable tool for better simulating the formation and evolution of SOA where SOA precursors are grouped by their volatility. This is done in order to avoid the computational cost of simulating possibly hundreds of atmospheric organic species involved in SOA formation. The accuracy of this framework relies upon the accuracy of the volatility distribution of the oxidation products of volatile organic compounds (VOCs) used to represent SOA formation. However, the volatility distribution of SOA-forming vapours remains inadequately constrained within global climate models, leading to uncertainties in the predicted aerosol mass loads and climate impacts. This study presents the results from simulations using a process-scale particle growth model and a global climate model, illustrating how uncertainties in the volatility distribution of biogenic SOA precursor gases affect the simulated cloud condensation nuclei (CCN). We primarily focused on the volatility of oxidation products derived from monoterpenes as they represent the dominant class of VOCs emitted by boreal trees. Our findings reveal that the particle growth rate and their survival to CCN sizes, as simulated by the process-scale model, are highly sensitive to uncertainties in the volatilities of condensing organic vapours. Interestingly, we note that this high sensitivity is less pronounce in global-scale model simulations as the CCN concentration and cloud droplet number concentration (CDNC) simulated in the global model remain insensitive to a 1-order-of-magnitude shift in the volatility distribution of organics. However, a notable difference arises in the SOA mass concentration as a result of volatility shifts in the global model. Specifically, a 1-order-of-magnitude decrease in volatility corresponds to an approximate 13 % increase in SOA mass concentration, while a 1-order-of-magnitude increase results in a 9 % decrease in SOA mass concentration over the boreal region. SOA mass and CCN concentrations are found to be more sensitive to the uncertainties associated with the volatility of semi-volatile compounds, with saturation concentrations of 10 -1 µgm-3 or higher, than the low-volatility compounds. This finding underscores the importance of having a higher resolution in the semi-volatile bins, especially in global models, to accurately capture SOA formation. Furthermore, the study highlights the importance of a better representation of saturation concentration values for volatility bins when employing a reduced number of bins in a global-scale model. A comparative analysis between a finely resolved nine-bin VBS setup and a simpler three-bin VBS setup highlights the significance of these choices. The study also indicates that radiative forcing attributed to changes in SOA over the boreal forest region is notably more sensitive to the volatility distribution of semi-volatile compounds than low-volatility compounds. In the three-bin VBS setup, a 10-fold decrease in the volatility of the highest-volatility bin results in a shortwave instantaneous radiative forcing (IRFari) of - 0.2 ± 0.10 Wm-2 and an effective radiative forcing (ERF) of + 0.8 ± 2.24 Wm-2 , while a 10-fold increase in volatility leads to an IRFari of + 0.05 ± 0.04 Wm-2 and an ERF of + 0.45 ± 2.3 Wm-2 over the boreal forest region. These findings underscore the critical need for a more accurate representation of semi-volatile compounds within global-scale models to effectively capture the aerosol loads and the subsequent climate effects. [ABSTRACT FROM AUTHOR]

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 , 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 CO 2 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 CO 2 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 CO 2 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 CO 2 , 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. [ABSTRACT FROM AUTHOR]

For over 6 months, the 2014–2015 effusive eruption at Holuhraun, Iceland, injected considerable amounts of sulfur dioxide (SO2) into the lower troposphere with a daily rate of up to one-third of the global emission rate, causing extensive air pollution across Europe. The large injection of SO2 , which oxidises to form sulfate aerosol (SO42-), provides a natural experiment offering an ideal opportunity to scrutinise state-of-the-art general circulation models' (GCMs) representation of aerosol–cloud interactions (ACIs). Here we present Part 1 of a two-part model inter-comparison using the Holuhraun eruption as a framework to analyse ACIs. We use SO2 retrievals from the Infrared Atmospheric Sounding Interferometer (IASI) instrument and ground-based measurements of SO2 and SO42- mass concentrations across Europe, in conjunction with a trajectory analysis using the Hybrid Single Particle Lagrangian Integrated Trajectory (HYSPLIT) model, to assess the spatial and chemical evolution of the volcanic plume as simulated by five GCMs and a chemical transport model (CTM). IASI retrievals of plume altitude and SO2 column load reveal that the volcanic perturbation is largely contained within the lower troposphere. Compared to the satellite observations, the models capture the spatial evolution and vertical variability of the plume reasonably well, although the models often overestimate the plume altitude. HYSPLIT trajectories are used to attribute to Holuhraun emissions 111 instances of elevated sulfurous surface mass concentrations recorded at European Monitoring and Evaluation Programme (EMEP) stations during September and October 2014. Comparisons with the simulated concentrations show that the modelled ratio of SO2 to SO42- during these pollution episodes is often underestimated and overestimated for the young and mature plume, respectively. Models with finer vertical resolutions near the surface are found to better capture these elevated sulfurous ground-level concentrations. Using an exponential function to describe the decay of observed surface mass concentration ratios of SO2 to SO42- with plume age, the in-plume oxidation rate constant is estimated as 0.032 ± 0.002 h-1 (1.30 ± 0.08 d e -folding time), with a near-vent ratio of 25 ± 5 (µgm-3 of SO2 / µgm-3 of SO42-). The majority of the corresponding derived modelled oxidation rate constants are lower than the observed estimate. This suggests that the representation of the oxidation pathway/s in the simulated plumes is too slow. Overall, despite their coarse spatial resolutions, the six models show reasonable skill in capturing the spatial and chemical evolution of the Holuhraun plume. This capable representation of the underlying aerosol perturbation is essential to enable the investigation of the eruption's impact on ACIs in the second part of this study. [ABSTRACT FROM AUTHOR]

Secondary organic aerosol (SOA) constitutes an important component of atmospheric particulate matter, with substantial influence on air quality, human health and the global climate. Volatility basis set (VBS) framework has provided a valuable tool for better simulating the formation and evolution of SOA where SOA precursors are grouped by their volatility. This is done in order to avoid the computational cost of simulating possibly hundreds of atmospheric organic species involved in SOA formation. The accuracy of this framework relies upon the accuracy of the volatility distribution of the oxidation products of volatile organic compounds (VOCs) used to represent SOA formation. However, the volatility distribution of SOA forming vapours remains inadequately constrained within global climate models, leading to uncertainties in the predicted aerosol mass loads and climate impacts. This study presents the results from simulations using a process-scale particle growth model and global climate model, illustrating how uncertainties in the volatility distribution of biogenic SOA precursor gases affects the simulated cloud condensation nuclei (CCN). We primarily focused on the volatility of oxidation products derived from monoterpenes as they represent the dominant class of VOCs emitted by boreal trees. Our findings reveal that the particle growth rate and their survival to CCN sizes, as simulated by the process scale model, are highly sensitive to uncertainties in the volatilities of condensing organic vapours. Interestingly, we note that this high sensitivity is less pronounce in global scale model simulations, as the CCN concentration and cloud droplet number concentration (CDNC) simulated in the global model remain insensitive to a one order of magnitude shift in the volatility distribution of organics. However, a notable difference arises in the SOA mass concentration as a result of volatility shifts in the global model. Specifically, a one order of magnitude decrease in volatility corresponds to an approximate 13% increase in SOA mass concentration, while, a one order of magnitude increase results in a 9% decrease in SOA mass concentration over the boreal region. SOA mass and CCN concentrations are found to be more sensitive to the uncertainties associated with the volatility of semi-volatile compounds than the low-volatile compounds. Furthermore, the study highlights the importance of a better representation of saturation concentration values for volatility bins when employing a reduced number of bins in a global scale model. A comparative analysis between a finely resolved 9-bin VBS setup and a simpler 3-bin VBS setup highlights the significance of these choices. The study also indicates that radiative forcing attributed to changes in SOA is notably more sensitive to the volatility distribution of semi-volatile compounds than low-v olatile compounds. In the 3-bin VBS setup, a ten-fold decrease in volatility of the highest volatility bin results in a shortwave instantaneous radiative forcing (IRFari) of -0.2 ± 0.10 Wm-2 and an effective radiative forcing (ERF) of +0.8 ± 2.24 Wm-2, while a ten-fold increase in volatility leads to an IRFari of +0.05 ± 0.04 Wm-2 and ERF of +0.45 ± 2.3 Wm-2. These findings underscore the critical need for a more accurate representation of semi-volatile compounds within global scale models to effectively capture the aerosol loads and the subsequent climate effects. [ABSTRACT FROM AUTHOR]

This is the second of two papers where we study the dependency of the impacts of stratospheric sulfur injections on the used model and injection strategy. 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, are implemented consistently into EC-Earth, MPI-ESM and CESM Earth System Models to simulate the climate impacts of different injection rates ranging from 2 to 100 Tg(S)yr−1. Two sets of simulations were simulated with the three ESMs: 1) Regression simulations, where abrupt change in CO2 concentration or stratospheric aerosols over preindustrial conditions were applied to quantify global mean fast temperature independent climate responses and quasi-linear dependence on temperature and 2) equilibrium simulations, where radiative forcing of aerosol injections with various magnitudes compensate the corresponding radiative forcing of CO2 enhancement to study the dependence of precipitation on the injection magnitude; the latter also allow to explore the regional climatic responses. Large differences in SALSA and M7 simulated radiative forcings in Part 1 translated into large differences in the estimated surface temperature and precipitation changes in ESM simulations: e.g. 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 5.2 K change. In equilibrium simulation, where aerosol injections were used to compensate for radiative forcing of 500 ppm atmospheric CO2 concentration, global mean precipitation reduction varied between models from -0.7 to - 2.4 %. These precipitation changes can be explained by the fast precipitation response due to radiation changes caused by the stratospheric aerosols and CO2 because global mean fast precipitation response is rather negatively correlated with global mean absorbed radiation. Our study shows that estimating the impact of stratospheric aerosol injection on climate is not straightforward. This is because the capability of the sulfate layer to reflect solar radiation and absorb LW 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. [ABSTRACT FROM AUTHOR]

Sulfate aerosol in the stratosphere is an important climate driver, causing solar dimming in the years after major volcanic eruptions. Hence, a growing number of general circulation models are adapting interactive sulfur and aerosol schemes to improve the representation of relevant chemical processes and associated feedbacks. However, uncertainties of these schemes are not well constrained. Stratospheric sulfate is modulated by natural emissions of sulfur-containing species, including volcanic eruptive, and anthropogenic emissions. Model intercomparisons have examined the effects of volcanic eruptions, whereas the background conditions of the sulfur cycle have not been addressed in a global model intercomparison project. Assessing background conditions in global models allows us to identify model discrepancies as they are masked by large perturbations such as volcanic eruptions, yet may still matter in the aftermath of such a disturbance. Here, we analyze the atmospheric burden, seasonal cycle, and vertical and meridional distribution of the main sulfur species among nine global atmospheric aerosol models that are widely used in the stratospheric aerosol research community. We use observational and reanalysis data to evaluate model results. Overall, models agree that the three dominant sulfur species in terms of burdens (sulfate aerosol, OCS, and SO2) make up about 98 % of stratospheric sulfur and 95 % of tropospheric sulfur. However, models vary considerably in the partitioning between these species. Models agree that anthropogenic emission of SO2 strongly affects the sulfate aerosol burden in the Northern Hemispheric troposphere, while its importance is very uncertain in other regions. The total deposition of sulfur varies among models, deviating by a factor of two, but models agree that sulfate aerosol is the main form in which sulfur is deposited. Additionally, the partitioning between wet and dry deposition fluxes is highly model dependent. We investigate the areas of greatest variability in the sulfur species burdens and find that inter-model variability is low in the tropics and increases towards the poles. Seasonality in the southern hemisphere is depicted very similar among models. Differences are largest in the dynamically active northern hemispheric extratropical region, hence some of the differences could be attributed to the differences in the representation of the stratospheric circulation among underlying general circulation models. This study highlights that the differences in the atmospheric sulfur budget among the models arise from the representation of both chemical and dynamical processes, whose interplay complicates the bias attribution. Several problematic points identified for individual models are related to the specifics of the chemistry schemes, model resolution, and representation of cross-tropopause transport in the extratropics. Further model intercomparison research is needed focusing on the clarification of the reasons for biases, given also the importance of this topic for the stratospheric aerosol injection studies. [ABSTRACT FROM AUTHOR]

For over 6-months, the 2014–2015 effusive eruption at Holuhraun, Iceland injected considerable amounts of sulphur dioxide (SO2) into the lower troposphere with a daily rate of up to one-third of the global emission rate causing extensive air pollution across Europe. The large injection of SO2, which oxidises to form sulphate aerosol (SO42−), provides a natural experiment offering an ideal opportunity to scrutinise state-of-the-art general circulation models (GCMs) representation of aerosol-cloud interactions (ACIs). Here we present Part 1 of a two-part model inter-comparison using the Holuhraun eruption as a framework to analyse ACIs. We use SO2 retrievals from the Infrared Atmospheric Sounding Interferometer (IASI) instrument and ground-based measurements of SO2 and SO42− mass concentrations across Europe in conjunction with trajectory analysis using the Hybrid Single Particle Lagrangian Integrated Trajectory (HYSPLIT) model to assess the spatial and chemical evolution of the volcanic plume as simulated by 5 GCMs and a chemical transport model (CTM). IASI retrievals of plume altitude and SO2 column load reveal that the volcanic perturbation is largely contained within the lower troposphere and that the spatial evolution and vertical variability of the plume is reasonably well captured by the models, although the models underestimate the mean plume altitude. HYSPLIT trajectories are used to attribute to Holuhraun emissions 184 instances of elevated sulphurous surface mass concentrations recorded at 22 air monitoring stations across Europe. Comparisons with the simulated concentrations show that the models underestimate the elevated SO2 concentrations observed at stations closer to Holuhraun whilst overestimating those observed further away. Using a biexponential function to describe the decay of observed surface mass concentration ratios of SO2-to-SO42− with plume age, in-plume gas-phase and aqueous-phase oxidation rates are estimated as 0.031 ± 0.002 h−1 and 0.22 ± 0.16 h−1 respectively with a near-vent ratio of 31 ± 4 [μgm−3 of SO2 / ugm−3 of SO42−]. The derived gas-phase oxidation rates from the models are all lower than the observed estimate, whilst the majority of the aqueous-phase oxidation rates agree with the observed rate. This suggests that the simulated plumes capture the observed chemical behaviour in the young plume (when aqueous-phase oxidation is dominant), yet not in the mature plume (when gas-phase oxidation is dominant). Overall, despite their coarse resolution, the 6 models show reasonable skill in capturing the spatial and chemical evolution of the Holuhraun plume which is essential when exploring the eruption impact on ACIs in the second part of this study. [ABSTRACT FROM AUTHOR]

Recent model inter-comparison studies highlighted model discrepancies in reproducing the climatic impacts of large explosive volcanic eruptions, calling into question the reliability of global aerosol model simulations for future scenarios. Here, we analyse the simulated evolution of the stratospheric aerosol plume following the well observed June 1991 Mt. Pinatubo eruption by six interactive stratospheric aerosol microphysics models in comparison to a range of observational data sets. Our primary focus 5 is on the uncertainties regarding initial SO2 emission following the Pinatubo eruption in 1991, as prescribed in the Historical Eruptions SO2 Emission Assessment experiments (HErSEA), in the framework of the Interactive Stratospheric Aerosol Model Intercomparison Project (ISA-MIP). Six global models with interactive aerosol microphysics took part in this study: ECHAM6-SALSA, EMAC, ECHAM5-HAM, SOCOL-AERv2, ULAQ-CCM and UM-UKCA. Model simulations are performed by varying SO2 injection amount (ranging between 5 and 10 Tg-S), and the altitude of injection (between 18-25 km). We find that the common and main weakness among all the models is that they can not reproduce the persistence of the sulfate aerosols in the stratosphere. Most models show a stronger transport towards the extratropics in the northern hemisphere, at the expense of the observed tropical confinement, suggesting a much weaker subtropical barrier in all the models, that results in a shorter e-folding time compared to the observations. Moreover, the simulations in which more than 5 Tg-S of SO2 are injected show a large surface area density a few months after the eruption compared to the values measured in the tropics and the in-situ measurements over Laramie. This results in an overestimation of the number of particles globally during the build-up phase and an underestimation in the Southern Hemisphere, which draws attention to the importance of including processes as the ash injection and the eruption of Cerro Hudson. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]