Stratospheric Aerosol Optical Depth Research Articles

Evolution of the Climate Forcing During the Two Years After the Hunga Tonga‐Hunga Ha'apai Eruption

AbstractWe calculate the climate forcing for the 2 ys after the 15 January 2022, Hunga Tonga‐Hunga Ha'apai (Hunga) eruption. We use satellite observations of stratospheric aerosols, trace gases and temperatures to compute the tropopause radiative flux changes relative to climatology. Overall, the net downward radiative flux decreased compared to climatology. The Hunga stratospheric water vapor anomaly initially increases the downward infrared radiative flux, but this forcing diminishes as the anomaly disperses. The Hunga aerosols cause a solar flux reduction that dominates the net flux change over most of the 2 yrs period. Hunga induced temperature changes produce a decrease in downward long‐wave flux. Hunga induced ozone reduction increases the short‐wave downward flux creating small sub‐tropical increase in total flux from mid‐2022 to 2023. By the end of 2023, most of the Hunga induced radiative forcing changes have disappeared. There is some disagreement in the satellite measured stratospheric aerosol optical depth (SAOD) observations which we view as a measure of the uncertainty; however, the SAOD uncertainty does not alter our conclusion that, overall, aerosols dominate the radiative flux changes.

The Recovery and Re-Calibration of a 13-Month Aerosol Extinction Profiles Dataset from Searchlight Observations from New Mexico, after the 1963 Agung Eruption

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

The 2019 Raikoke eruption as a testbed used by the Volcano Response group for rapid assessment of volcanic atmospheric impacts

Abstract. ​​​​​​​The 21 June 2019 Raikoke eruption (48° N, 153° E) generated one of the largest amounts of sulfur emission to the stratosphere since the 1991 Mt. Pinatubo eruption. Satellite measurements indicate a consensus best estimate of 1.5 Tg for the sulfur dioxide (SO2) injected at an altitude of around 14–15 km. The peak Northern Hemisphere (NH) mean 525 nm stratospheric aerosol optical depth (SAOD) increased to 0.025, a factor of 3 higher than background levels. The Volcano Response (VolRes) initiative provided a platform for the community to share information about this eruption which significantly enhanced coordination efforts in the days after the eruption. A multi-platform satellite observation subgroup formed to prepare an initial report to present eruption parameters including SO2 emissions and their vertical distribution for the modeling community. It allowed us to make the first estimate of what would be the peak in SAOD 1 week after the eruption using a simple volcanic aerosol model. In this retrospective analysis, we show that revised volcanic SO2 injection profiles yield a higher peak injection of the SO2 mass. This highlights difficulties in accurately representing the vertical distribution for moderate SO2 explosive eruptions in the lowermost stratosphere due to limited vertical sensitivity of the current satellite sensors (±2 km accuracy) and low horizontal resolution of lidar observations. We also show that the SO2 lifetime initially assumed in the simple aerosol model was overestimated by 66 %, pointing to challenges for simple models to capture how the life cycle of volcanic gases and aerosols depends on the SO2 injection magnitude, latitude, and height. Using a revised injection profile, modeling results indicate a peak NH monthly mean SAOD at 525 nm of 0.024, in excellent agreement with observations, associated with a global monthly mean radiative forcing of −0.17 W m−2 resulting in an annual global mean surface temperature anomaly of −0.028 K. Given the relatively small magnitude of the forcing, it is unlikely that the surface response can be dissociated from surface temperature variability.

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.

Unexpectedly rapid aerosol formation in the Hunga Tonga plume.

The Hunga Tonga-Hunga Ha'apai (HT-HH) volcanic eruptions on January 13 and 15, 2022, produced a plume with the highest signal in stratospheric aerosol optical depth observed since the eruption of Mt. Pinatubo in 1991. Suites of balloon-borne instruments on a series of launches from Réunion Island intercepted the HT-HH plume between 7 and 10 d of the eruptions, yielding observations of the aerosol number and size distribution and sulfur dioxide (SO2) and water vapor (H2O) concentrations. The measurements reveal an unexpected abundance of large particles in the plume, constrain the total sulfur injected to approximately 0.2 Tg, provide information on the altitude of the injection, and indicate that the formation of sulfuric acid aerosol was complete within 3 wk. Large H2O enhancements contributed as much as ~30% to ambient aerosol surface area and likely accelerated SO2 oxidation and aerosol formation rates in the plume to approximately three times faster than under normal stratospheric conditions.

Short- and long-term stratospheric impact of smoke from the 2019–2020 Australian wildfires

Abstract. At the end of December 2019 and beginning of 2020, massive firestorms in Australia formed pyrocumulonimbus clouds (pyroCbs) that acted like enormous smokestacks, pumping smoke to the upper troposphere and stratosphere. We study the smoke with data from four satellite-based sensors: the aerosol observation platforms CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization), OMPS-LP (Ozone Mapping and Profiler Suite Limb Profiler), and OMPS-NM (Ozone Mapping and Profiler Suite Nadir Mapper) and water vapor retrievals from MLS (Microwave Limb Sounder). Smoke was lofted to the upper troposphere and stratosphere during two events and spread almost exclusively within the extratropics. Smoke from the first event, starting 29 December, was injected directly into the stratosphere by pyroCbs, causing a rapid initial increase in AOD (aerosol optical depth). CALIOP identifies a rapid decline in this stratospheric smoke (half-life: 10 d), not captured in previous studies of the Australian fires, indicating photochemical processing of organic aerosol. This decay rate is in line with model predictions of mid-tropospheric organic aerosol loss by photolytic removal and is in agreement with our estimates of decay rates after the North American fires in August 2017. PyroCbs from the second event, 4 January, injected small amounts of smoke directly into the stratosphere. Large amounts of smoke were injected to the upper troposphere, from where it ascended into the stratosphere during several weeks, forming a second peak in the aerosol load. Hence, we find that pyroCbs can impact the stratospheric aerosol load both via direct injection to the stratosphere and through injection of smoke to the upper troposphere from where the smoke ascends into the stratosphere. The stratospheric AOD from the second-event fires decreased more slowly than the AOD from the first event, likely due to a combination of photolytic loss starting already in the troposphere and continued supply of smoke from the upper troposphere offsetting the loss rate. Together these injections yielded a major increase in the aerosol load for almost 1 year.

Climate, Variability, and Climate Sensitivity of “Middle Atmosphere” Chemistry Configurations of the Community Earth System Model Version 2, Whole Atmosphere Community Climate Model Version 6 (CESM2(WACCM6))

AbstractSimulating whole atmosphere dynamics, chemistry, and physics is computationally expensive. It can require high vertical resolution throughout the middle and upper atmosphere, as well as a comprehensive chemistry and aerosol scheme coupled to radiation physics. An unintentional outcome of the development of one of the most sophisticated and hence computationally expensive model configurations is that it often excludes a broad community of users with limited computational resources. Here, we analyze two configurations of the Community Earth System Model Version 2, Whole Atmosphere Community Climate Model Version 6 (CESM2(WACCM6)) with simplified “middle atmosphere” chemistry at nominal 1 and 2° horizontal resolutions. Using observations, a reanalysis, and direct model comparisons, we find that these configurations generally reproduce the climate, variability, and climate sensitivity of the 1° nominal horizontal resolution configuration with comprehensive chemistry. While the background stratospheric aerosol optical depth is elevated in the middle atmosphere configurations as compared to the comprehensive chemistry configuration, it is comparable among all configurations during volcanic eruptions. For any purposes other than those needing an accurate representation of tropospheric organic chemistry and secondary organic aerosols, these simplified chemistry configurations deliver reliable simulations of the whole atmosphere that require 35% and 86% fewer computational resources at nominal 1 and 2° horizontal resolution, respectively.

Volatile emissions from past eruptions at La Soufrière de Guadeloupe (Lesser Antilles): insights into degassing processes and atmospheric impacts

Volatiles exert a critical control on volcanic eruption style and in turn impact the near source environment and global climate. La Soufrière de Guadeloupe in the Lesser Antilles has been experiencing volcanic unrest since 1992, increasing to a peak in 2018. The lack of data available on volatiles from past eruptions, and the well-developed hydrothermal system makes understanding deep-released volatile behaviour challenging. In this study, we analyse new melt inclusions and shed light on the volatile lifecycle and impacts at La Soufrière de Guadeloupe. We focus on four eruptions: 1657 CE (Vulcanian), 1010 CE (Plinian), 341 CE (Strombolian) and 5680 BCE (Plinian), and compare to the well-studied 1530 CE (Sub-Plinian) eruption. The maximum volatile content of these eruption melt inclusions are: 4.42 wt% H2O, 1700 CO2 ppm, 780 ppm S, 0.36 wt% Cl and 680 ppm F. We observe a decrease in S content over time indicating the whole system is evolving by early separation of FeS, resulting in a lower S content in younger magma. Using the CHOSETTO v1 model, we modelled degassing paths related to decompression at low pressures, suggesting the majority of S degassing has occurred during magma ascent. We also calculate the SO2 emissions using the petrologic method, and while the 1657 CE, 1530 CE and 341 CE eruptions have negligible emissions (0.0001–0.001 Mt of SO2), the 1010 CE and 5680 BCE eruptions (0.2 Mt and 0.3 Mt of SO2, respectively) are greater. Using the SO2 emissions and plume height, we calculated the climate forcing associated with each event. The 1010 CE and 5680 BCE Plinian eruptions produced a peak global mean stratospheric aerosol optical depth (SAOD) of 0.0055 and 0.0062, respectively. This suggests, that even the largest eruptions of La Soufrière de Guadeloupe did not exert a significant climate forcing individually, but are important contributors to the volcanic stratospheric sulfate aerosol background resulting from relatively moderate but frequent explosive eruptions. Overall, this study provides new insights into degassing processes and climate forcing not only at La Soufrière de Guadeloupe, but also for other basaltic-andesitic, magmatic-hydrothermal systems. These new constraints are vital particularly if the volcano is currently in a state of unrest and will contribute to improving monitoring crisis management and long-term planning.

Climate Projections Very Likely Underestimate Future Volcanic Forcing and Its Climatic Effects

AbstractStandard climate projections represent future volcanic eruptions by a constant forcing inferred from 1850 to 2014 volcanic forcing. Using the latest ice‐core and satellite records to design stochastic eruption scenarios, we show that there is a 95% probability that explosive eruptions could emit more sulfur dioxide (SO2) into the stratosphere over 2015–2100 than current standard climate projections (i.e., ScenarioMIP). Our simulations using the UK Earth System Model with interactive stratospheric aerosols show that for a median future eruption scenario, the 2015–2100 average global‐mean stratospheric aerosol optical depth (SAOD) is double that used in ScenarioMIP, with small‐magnitude eruptions (<3 Tg of SO2) contributing 50% to SAOD perturbations. We show that volcanic effects on large‐scale climate indicators, including global surface temperature, sea level and sea ice extent, are underestimated in ScenarioMIP because current climate projections do not fully account for the recurrent frequency of volcanic eruptions of different magnitudes.

Quantification of tropical monsoon precipitation changes in terms of interhemispheric differences in stratospheric sulfate aerosol optical depth

Stratospheric Aerosol Geoengineering (SAG) is one of the solar geoengineering approaches that have been proposed to offset some of the impacts of anthropogenic climate change. Past studies have shown that SAG may have adverse impacts on the global hydrological cycle. Using a climate model, we quantify the sensitivity of the tropical monsoon precipitation to the meridional distribution of volcanic sulfate aerosols prescribed in the stratosphere in terms of the changes in aerosol optical depth (AOD). In our experiments, large changes in summer monsoon precipitation in the tropical monsoon regions are simulated, especially over the Indian region, in association with meridional shifts in the location of the intertropical convergence zone (ITCZ) caused by changes in interhemispheric AOD differences. Based on our simulations, we estimate a sensitivity of − 1.8° ± 0.0° meridional shift in global mean ITCZ and a 6.9 ± 0.4% reduction in northern hemisphere (NH) monsoon index (NHMI; summer monsoon precipitation over NH monsoon regions) per 0.1 interhemispheric AOD difference (NH minus southern hemisphere). We also quantify this sensitivity in terms of interhemispheric differences in effective radiative forcing and interhemispheric temperature differences: 3.5 ± 0.3% change in NHMI per unit (Wm−2) interhemispheric radiative forcing difference and 5.9 ± 0.4% change per unit (°C) interhemispheric temperature difference. Similar sensitivity estimates are also made for the Indian monsoon precipitation. The establishment of the relationship between interhemispheric AOD (or radiative forcing) differences and ITCZ shift as discussed in this paper will further facilitate and simplify our understanding of the effects of SAG on tropical monsoon rainfall.

Volcanic Drivers of Stratospheric Sulfur in GFDL ESM4

AbstractStratospheric injections of sulfur dioxide from major volcanic eruptions perturb the Earth's global radiative balance and dominate variability in stratospheric sulfur loading. The atmospheric component of the GFDL Earth System Model (ESM4.1) uses a bulk aerosol scheme and previously prescribed the distribution of aerosol optical properties in the stratosphere. To quantify volcanic contributions to the stratospheric sulfur cycle and the resulting climate impact, we modified ESM4.1 to simulate stratospheric sulfate aerosols prognostically. Driven by explicit volcanic emissions of aerosol precursors and non‐volcanic sources, we conduct ESM4.1 simulations from 1989 to 2014, with a focus on the Mt. Pinatubo eruption. We evaluate our interactive representation of the stratospheric sulfur cycle against data from Moderate Resolution Imaging Spectroradiometer, Multi‐angle Imaging SpectroRadiometer, Advanced Very High Resolution Radiometer, High Resolution Infrared Radiation Sounder, and Stratospheric Aerosol and Gas Experiment II. To assess the key processes associated with volcanic aerosols, we performed a sensitivity analysis of sulfate burden from the Mt. Pinatubo eruption by varying injection heights, emission amount, and stratospheric sulfate's dry effective radius. We find that the simulated stratospheric sulfate mass burden and aerosol optical depth in the model are sensitive to these parameters, especially volcanic SO2 injection height, and the optimal combination of parameters depends on the metric we evaluate.

The effect of ash, water vapor, and heterogeneous chemistry on the evolution of a Pinatubo-size volcanic cloud

Abstract. We employ the ECHAM5/MESSy2 atmospheric chemistry general circulation model (EMAC) that incorporates calculations of gas-phase and heterogeneous chemistry coupled with the ozone cycle and aerosol formation, transport, and microphysics to calculate the 1991 Pinatubo volcanic cloud. We considered simultaneous injections of SO2, volcanic ash, and water vapor. We conducted multiple ensemble simulations with different injection configurations to test the evolution of SO2, SO42-, ash masses, stratospheric aerosol optical depth, surface area density (SAD), and the stratospheric temperature response against available observations. We found that the volcanic cloud evolution is sensitive to the altitude where volcanic debris is initially injected and the initial concentrations of the eruption products that affect radiative heating and lofting of the volcanic cloud. The numerical experiments with the injection of 12 Mt SO2, 75 Mt of volcanic ash, and 150 Mt of water vapor at 20 km show the best agreement with the observation aerosol optical depth and stratospheric temperature response. Volcanic water injected by eruptive jet and/or intruding through the tropopause accelerates SO2 oxidation. But the mass of volcanic water retained in the stratosphere is controlled by the stratospheric temperature at the injection level. For example, if volcanic materials are released in the cold point above the tropical tropopause, most of the injected water freezes and sediments as ice crystals. The water vapor directly injected into the volcanic cloud increases the SO42- mass and stratospheric aerosol optical depth by about 5 %. The coarse ash comprises 98 % of the ash injected mass. It sediments within a few days, but aged submicron ash could stay in the stratosphere for a few months providing SAD for heterogeneous chemistry. The presence of ash accelerates the SO2 oxidation by 10 %–20 % due to heterogeneous chemistry, radiative heating, lofting, and faster dispersion of volcanic debris. Ash aging affects its lifetime and optical properties, almost doubling the ash radiative heating. The 2.5-year simulations show that the stratospheric temperature anomalies forced by radiative heating of volcanic debris in our experiments with the 20 km injection height agree well with observations and reanalysis data. This indicates that the model captures the long-term evolution and climate effect of the Pinatubo volcanic cloud. The volcanic cloud's initial lofting, facilitated by ash particles' radiative heating, controls the oxidation rate of SO2. Ash accelerates the formation of the sulfate layer in the first 2 months after the eruption. We also found that the interactive calculations of OH and heterogeneous chemistry increase the volcanic cloud sensitivity to water vapor and ash injections. All those factors must be accounted for in modeling the impact of large-scale volcanic injections on climate and stratospheric chemistry.

Stratospheric Aerosol Characteristics from the 2017–2019 Volcanic Eruptions Using the SAGE III/ISS Observations

In recent years (2017–2019), several moderate volcanic eruptions and wildfires have perturbed the stratospheric composition and concentration with distinct implications on radiative forcing and climate. The Stratospheric Aerosol and Gas Experiment III instruments onboard the International Space Station (SAGE III/ISS) have been providing aerosol extinction coefficient (EC) profiles at multiple wavelengths since June 2017. In this study, a method to invert the spectral stratospheric aerosol optical depth (sAOD) or EC values from SAGE III/ISS (to retrieve the number/volume size distributions and other microphysical properties) is presented, and the sensitivity of these retrievals is evaluated. It was found that the retrievals are strongly dependent on the choices of wavelengths, which in turn determine the shapes of the calculated curves. Further, we examine the changes in stratospheric aerosol spectral behavior, size distribution properties, time evolution (growth/decay) characteristics associated with subsequent moderate volcanic eruptions, namely, Ambae (15∘S, 167∘E; April and July 2018), Raikoke (48∘N, 153∘E; June 2019), and Ulawun (5∘S, 151∘E; June and August 2019), in different spatial regions. The observational period was classified with reference to Ambae eruptions into four phases (pre-Ambae, Ambae1, Ambae2, and post-Ambae). The pre-Ambae and post-Ambe periods comprise the 2017 Canadian fires and 2019 Raikoke/Ulawun eruptions, respectively. The spectral dependence of sAOD was comparable and lowest during the pre-Ambae and Ambae1 periods in all regions. The number concentration at the principal mode radius (between 0.07 and 0.2 μm) was observed to be higher during the Ambae2 period over the Northern Hemisphere (NH). The rate of change (growth/decay) in the sAOD on a global scale resembled the changes in the Southern Hemisphere (SH), unlike the time-lag-associated changes in the NH. These differences could be attributed to the prevailing horizontal and vertical dispersion mechanisms in the respective regions. Lastly, the radiative forcing estimates of Ambae and Raikoke/Ulawun eruptions, as reported in recent studies, was discussed by taking clues from other major and moderate eruptions to gain insight on their role in climate change.

Perturbations in stratospheric aerosol evolution due to the water-rich plume of the 2022 Hunga-Tonga eruption

The January 2022 Hunga Tonga-Hunga Ha’apai volcanic eruption injected a relatively small amount of sulfur dioxide, but significantly more water into the stratosphere than previously seen in the modern satellite record. Here we show that the large amount of water resulted in large perturbations to stratospheric aerosol evolution. Our climate model simulation reproduces the observed enhanced water vapor at pressure levels ~30 hPa for three months. Compared with a simulation without a water injection, this additional source of water vapor increases hydroxide, which halves the sulfur dioxide lifetime. Subsequent coagulation creates larger sulfate particles that double the stratospheric aerosol optical depth. A seasonal forecast of volcanic plume transport in the southern hemisphere indicates this eruption will greatly enhance the aerosol surface area and water vapor near the polar vortex until at least October 2022, suggesting that there will continue to be an impact of this eruption on the climate system.

Tracking the 2022 Hunga Tonga-Hunga Ha'apai Aerosol Cloud in the Upper and Middle Stratosphere Using Space-Based Observations.

On 15 January 2022, the submarine Hunga Tonga volcanic eruption lofted materials high into the upper stratosphere, reaching a record-breaking altitude of ∼58km, unprecedented in the satellite observations era. Within two weeks, the bulk of the injected material circulated the globe between 20-30km altitude, as observed by satellite instruments. We estimate that the stratospheric aerosol optical depth (sAOD) is the largest since the Pinatubo eruption and is at least twice as great as the sAOD after the 2015 Calbubo eruption despite the similar SO2 injection from that eruption. We use space-based observations to monitor the Hunga-Tonga volcanic plume evolution and transport at different altitudes as it circulates the globe. While the main aerosol layer remains trapped in the tropical pipe, small parts have already made it to both the northern and southern hemisphere poles by April, which is almost certain to influence this year's ozone hole.

Australian wildfires cause the largest stratospheric warming since Pinatubo and extends the lifetime of the Antarctic ozone hole

Global mean lower stratosphere temperatures rose abruptly in January 2020 reaching values not experienced since the early 1990s. Anomalously high lower stratospheric temperatures were recorded for 4 months at highly statistically significant levels. Here, we use a combination of satellite and surface-based remote sensing observations to derive a time-series of stratospheric biomass burning aerosol optical depths originating from intense SouthEastern Australian wildfires and use these aerosol optical depths in a state-of-the-art climate model. We show that the S.E. Australian wildfires are the cause of this lower stratospheric warming. We also investigate the radiatively-driven dynamical response to the observed stratospheric ozone perturbation and find a significant strengthening of the springtime Antarctic polar vortex suggesting that biomass burning aerosols play a significant role in the observed anomalous longevity of the ozone hole in 2020.

Columnar optical, microphysical and radiative properties of the 2022 Hunga Tonga volcanic ash plumes

The Hunga Tonga-Hunga Ha’apai eruption on January 15, 2022 was one of the most explosive volcanic eruptions of the 21st century and has attracted global attention. Here we show that large numbers of the volcanic aerosols from the eruption broke through the tropopause into the lower stratosphere, forming an ash plume with an overshooting top at 25–30 km altitude. In the four days following the eruption, the ash plume moved rapidly westward for nearly 10,000 km under stable stratospheric conditions characterized by strong tropical easterlies, weak meridional winds and weak vertical motion. The intrusion of the ash plume into the stratosphere resulted in a marked increase in atmospheric aerosol loading across northern Australia, with the aerosol optical depth (AOD) observed by satellites and sun-photometers peaking at 1.5 off the coast of northeastern Australia; these effects lasted for nearly three days. The ash plume was characterized by fine-mode particles clustered at a radius of about 0.26 µm, with an observed peak volume of 0.25 µm3 µm−2. The impact of the ash plume associated with the Hunga Tonga eruption on the stratospheric AOD and radiative balance in the tropical southern hemisphere is remarkable, with an observed volcanic-induced perturbation of the regional stratospheric AOD of up to 0.6. This perturbation largely explains an instantaneous bottom (top) of the atmosphere radiative forcing of −105.0 (−65.0) W m−2 on a regional scale.

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).

An approach to sulfate geoengineering with surface emissions of carbonyl sulfide

Abstract. Sulfate geoengineering (SG) methods based on lower stratospheric tropical injection of sulfur dioxide (SO2) have been widely discussed in recent years, focusing on the direct and indirect effects they would have on the climate system. Here a potential alternative method is discussed, where sulfur emissions are located at the surface or in the troposphere in the form of carbonyl sulfide (COS) gas. There are two time-dependent chemistry–climate model experiments designed from the years 2021 to 2055, assuming a 40 Tg-Syr-1 artificial global flux of COS, which is geographically distributed following the present-day anthropogenic COS surface emissions (SG-COS-SRF) or a 6 Tg-Syr-1 injection of COS in the tropical upper troposphere (SG-COS-TTL). The budget of COS and sulfur species is discussed, as are the effects of both SG-COS strategies on the stratospheric sulfate aerosol optical depth (∼Δτ=0.080 in the years 2046–2055), aerosol effective radius (0.46 µm), surface SOx deposition (+8.9 % for SG-COS-SRF; +3.3 % for SG-COS-TTL), and tropopause radiative forcing (RF; ∼-1.5 W m−2 in all-sky conditions in both SG-COS experiments). Indirect effects on ozone, methane and stratospheric water vapour are also considered, along with the COS direct contribution. According to our model results, the resulting net RF is −1.3 W m−2, for SG-COS-SRF, and −1.5 W m−2, for SG-COS-TTL, and it is comparable to the corresponding RF of −1.7 W m−2 obtained with a sustained injection of 4 Tg-Syr-1 in the tropical lower stratosphere in the form of SO2 (SG-SO2, which is able to produce a comparable increase of the sulfate aerosol optical depth). Significant changes in the stratospheric ozone response are found in both SG-COS experiments with respect to SG-SO2 (∼5 DU versus +1.4 DU globally). According to the model results, the resulting ultraviolet B (UVB) perturbation at the surface accounts for −4.3 % as a global and annual average (versus −2.4 % in the SG-SO2 case), with a springtime Antarctic decrease of −2.7 % (versus a +5.8 % increase in the SG-SO2 experiment). Overall, we find that an increase in COS emissions may be feasible and produce a more latitudinally uniform forcing without the need for the deployment of stratospheric aircraft. However, our assumption that the rate of COS uptake by soils and plants does not vary with increasing COS concentrations will need to be investigated in future work, and more studies are needed on the prolonged exposure effects to higher COS values in humans and ecosystems.

Influences of aerosols and thin cirrus clouds on GOSAT XCO2 and XCH4 using Total Carbon Column Observing Network, sky radiometer, and lidar data

ABSTRACT The column-averaged, dry air mole fractions of CO2 and CH4 (XCO2 and XCH4, respectively) were retrieved from short-wavelength infrared (SWIR) spectra observed by the Greenhouse gases Observing SATellite (GOSAT). Continuous measurements of SWIR spectra have been made via GOSAT since 2009, but there has been insufficient investigation of the effects of cirrus clouds and aerosols on the observations. In this work, we investigated the influences of aerosols and cirrus clouds on the differences between GOSAT observations and Total Carbon Column Observing Network (TCCON) data for XCO2 and XCH4 (ΔXCO2 and ΔXCH4) at three sites: Tsukuba and Saga in Japan, and Lauder in New Zealand. We used aerosol optical thickness (AOT), Angstrom exponents (AEs), and single scattering albedo (SSA), all obtained from sky radiometer observations, as well as vertical profiles of aerosols and thin cirrus clouds from lidar observations. Matchups were performed within ±0.1° latitude/longitude rectangular areas of each TCCON site, and within 30 min of the GOSAT overpass time. The results show a negative slope between ΔXCO2 and AOT at 500 nm determined from sky radiometer data at Tsukuba and Saga. The GOSAT XCO2 values tended to be lowered in the presence of cirrus clouds and dense boundary-layer aerosols. Moreover, a significant negative ΔXCO2 was observed at times of large AOTs that resulted from dust-like events. At Lauder, ΔXCO2 was negatively correlated with the AOT at 500 nm, although the AOT at this site was generally small. The mean ± standard deviation for ΔXCO2 and ΔXCH4 at Lauder are −0.80 ± 1.83 (ppm) and −5.27 ± 10.79 (ppb) with correlation coefficients r between GOSAT and TCCON of 0.94 and 0.83, respectively. Both ΔXCO2 and ΔXCH4 were significantly and negatively correlated with the AOT during Sep-Oct-Nov. In addition, stratospheric aerosols caused large negative biases of ΔXCO2 and ΔXCH4 at Lauder despite the small stratospheric aerosol optical depth at that site.