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A major strong sudden stratospheric warming (SSW) occurred in the Southern Hemisphere (SH) stratosphere in 2002 (hereafter referred to as SSW2002), which is one of the most unusual winters in the SH. Following several warmings, the polar vortex broke down in midwinter. Eastward-traveling waves and their interaction with quasi-stationary planetary waves played an important role during this event. This study analyzed the Japanese 55-year reanalysis (JRA-55) dataset to examine the SSW event that occurred in the SH in 2019 (hereafter referred to as SSW2019). In 2019, a rapid temperature increase and decelerated westerly winds were observed at the polar cap, but since there was no reversal of westerly winds to easterly winds at 60∘ S in the middle to lower stratosphere, the SSW2019 was classified as a minor warming event. The results showed that quasi-stationary planetary waves of zonal wavenumber 1 developed during the SSW2019. The strong vertical component of the Eliassen–Palm flux with zonal wavenumber 1 is indicative of pronounced propagation of planetary waves to the stratosphere. The wave driving in September 2019 was larger than that of the major SSW event in 2002. Major SSWs tend to accompany preceding minor warmings, preconditioning, which changes the zonal flow that weaken the polar night jet as seen in SSW2002. A similar preconditioning was hardly observed in SSW2019. The strong wave driving in SSW2019 occurred in high latitudes. Waveguides (i.e., positive values of the refractive index squared) were found at high latitudes in the upper stratosphere during the warming period, which provided favorable conditions for quasi-stationary planetary waves to propagate upward and poleward.

Large high-latitude explosive volcanic eruptions remain less well understood than their low-latitude counterparts, despite their potential for strong hemispheric climate impacts. Using the high-top coupled Earth system model CESM2-WACCM6 with prognostic stratospheric aerosols and chemistry, we simulate Pinatubo-magnitude Northern Hemisphere (NH) volcanic eruptions at 64° N. We show how the SO2 lifetime and growth of volcanic sulphate aerosols are strongly modulated by the initial state of the NH polar vortex for eruptions at this latitude. The resulting variability of the volcanic forcing is of comparable magnitude to its sensitivity to varying the plume composition, eruption season, and plume height. We compare the modelled volcanic sulphate deposition over the Greenland ice sheet to that assumed in current forcing reconstructions of past NH extratropical eruptions and provide a new model-based estimate of the magnitude and uncertainty of the transfer function used to reconstruct sulphur injections from such eruptions. Our results demonstrate the great potential for improvement in understanding and reconstructing the climatic impacts of NH high-latitude eruptions.

The Model Intercomparison Project on the climatic response to Volcanic forcing (VolMIP) is a protocol-driven international initiative under the umbrella of the sixth phase of the Coupled Model Intercomparison Project (CMIP6) aiming at coordinating the activities of different Research Institutes involved in numerical climate modelling focused on a multi-model assessment of climate models' performance under strong volcanic forcing conditions. The main objective of the initiative is to assess to what extent responses of the coupled ocean-atmosphere system to the same applied strong volcanic forcing are robustly simulated across state-of-the-art coupled climate models and identify the causes that limit robust simulated behavior, especially differences in their treatment of physical processes. To this purpose, four Tier-1 (mandatory) experiments branched into two main sets, named “volc-pinatubo” and “volc-long” were defined, together with eight more lower-priority experiments. Six years since the definition of the VolMIP protocol (Zanchettin et al., 2016), ensemble simulations of most of the mandatory VolMIP experiments have been completed and made publicly available through the Earth System Grid Federation open platform, with the first VolMIP results being currently published and several analyses in progress. The long turnover time between the experiment design, the integration of the simulations and the analysis of the output motivates an assessment of the overall effectiveness of the VolMIP strategy, particularly in the light of a possible second phase of the initiative.In this contribution, we will illustrate the status of the initiative, highlight its major achievements and discuss its future perspective in the light of emergent scientific questions regarding volcanically forced climate variability.Zanchettin, D., Khodri, M., Timmreck, C., Toohey, M., Schmidt, A., Gerber, E. P., Hegerl, G., Robock, A., Pausata, F. S. R., Ball, W. T., Bauer, S. E., Bekki, S., Dhomse, S. S., LeGrande, A. N., Mann, G. W., Marshall, L., Mills, M., Marchand, M., Niemeier, U., Poulain, V., Rozanov, E., Rubino, A., Stenke, A., Tsigaridis, K., and Tummon, F.: The Model Intercomparison Project on the climatic response to Volcanic forcing (VolMIP): experimental design and forcing input data for CMIP6, Geosci. Model Dev., 9, 2701–2719, https://doi.org/10.5194/gmd-9-2701-2016, 2

Studying impacts of past volcanic eruptions on climate and society relies on volcanology, paleo proxies and archaeological records next to climate model simulations. Here we newly study the control of varying meteorological conditions and eruption source parameters on the volcanic forcing. Simulating explosive tropical and extratropical Northern Hemisphere (NH) volcanic eruptions are carried out by co-injecting sulfur and halogens into the stratosphere with the CESM2(WACCM) model including aerosol, chemistry, climate, and earth system processes. We consider different initial meteorological conditions (ENSO, QBO, and polar vortex states) and varying eruption source parameters injecting 17 Tg and 200 Tg of SO2 together with scaled halogens, at 24 km altitude and 15° N and 64° N latitude, during January and July pre industrial 1850 conditions. Varying initial meteorological conditions reveal a similar large impact on the volcanic forcing (SO2, SO4, aerosol optical depth, halogens) as varying source parameters for both tropical and NH extratropical eruptions. Our results are compared with available model experiments from MAECHAM5-HAM. Consequences and uncertainties of volcanic forcing and responses to past and future eruptions are discussed.

“Solar Radiation Management” aims to mitigate global warming by either seeding aerosols into clouds to change their radiative properties and occurrence frequency, or injecting sulfur into the atmosphere to shield the Earth’s surface from incoming solar radiation. These approaches are inspired, among other things, by the effect of volcanic eruptions on the climate system.Here we provide a critical reassessment of a time period commonly referred to as the “Medieval Quiet Period”. For several centuries in early Medieval times (c. 750-1050 CE) the climate system was postulated to have been relatively unperturbed by natural climate forcing, resulting in a unique period of climate stability. We present evidence that just the opposite is true. In large parts of the Northern Hemisphere and in the Arctic, atmospheric aerosol loads were persistently high during this period as a result of increased volcanic activity, especially in Iceland.Our new insight is supported by evidence taken from an array of synchronized ice cores from Greenland with high time-resolution records of a large suite of trace elements, including volcanic volatiles such as sulfur, chlorine, fluorine, and heavy metals. We use crypto-tephra in ice cores to provenance the sources of many volcanic eruptions and sulfur isotopes (33S, 34S) to delineate if volcanic gas emissions occurred above or below the ozone layer.We define an “Iceland Active Period”, a time period of frequent and prolonged volcanic activity, producing persistently high levels in atmospheric aerosol burdens in the Northern Hemisphere Arctic’s preindustrial atmosphere lasting for decades to centuries. The frequency and cumulative amount of emissions of climate-impacting trace substances (e.g., sulfates, halogens, ash) is unprecedented in the late Holocene. It is exceeded at times only in the Anthropocene (since about 1900) and in the early-middle Holocene (e.g. during rapid deglaciation). We demonstrate that previous reconstructions of volcanic forcing used in PMIP3 and PMIP4 strongly underestimate volcanic aerosol emissions in the early Medieval and argue that this period should not be considered a reference climate state for the Common Era.Finally, we investigate possible aerosol-climate interactions following these eruptions using climate proxies and state-of-the-art chemistry climate models with prognostic stratospheric aerosols and chemistry.

Bromoform (CHBr3) is one of the most important precursors of atmospheric reactive bromine with an atmospheric lifetime of ~20 days. Natural production, being the main source of oceanic CHBr3, is high at the coasts and in open ocean upwelling regions due to production by macroalgae and phytoplankton. Although highly relevant for the future halogen burden and ozone layer in the stratosphere, the global bromoform production in the ocean and their emissions are still poorly constrained in observations and are mostly neglected in Earth System Model (ESM) climate projections. Here, we show first model results of fully coupled ocean-atmosphere bromoform interactions in the Norwegian ESM (NorESM) with the ocean model BLOM and the ocean biogeochemistry component iHAMOCC for the CMIP6 historical period from 1850 to 2014. Our results are validated using oceanic and atmospheric measurements listed in the HalOcAt (Halocarbons in the Ocean and Atmosphere) data base and show an overall good agreement with those observations in open ocean regions. The NorESM open ocean emissions of CHBr3 are higher than previously published emission estimates from bottom-up approaches. Moreover, the emissions are mainly positive (sea-to-air fluxes) driven by the oceanic production, sea surface temperature and wind speed, dependent on season and location. However, during low-productive winter seasons, model results also show local negative fluxes (air-to-sea fluxes) in high latitudes, suggesting some oceanic regions to be a sink of atmospheric bromoform. Driving factors will be shown for different case studies, e.g. the tropical West Pacific, which is a hot spot for oceanic bromine delivery to the stratosphere.

In the Northern Hemisphere, the mid-6th century was one of the coldest periods of the last 2000 years, as indicated by both proxy records and Earth System Model (ESM) simulations. This cold period was initiated by volcanic eruptions in 536 CE and 540 CE. Evidence from historical sources, archaeological findings, and proxy records suggests that the extent and severity of this volcanic induced cooling was spatially heterogeneous and that the effect on society resulted in adaptation and resilience at some locations, whereas social crisis has been indicated at others. Here, we study the effect of the volcanic double event in 536 CE and 540 CE on the climate and society in Scandinavia with a special focus on Southern Norway. Using an ensemble of Max Planck Institute ESM transient simulations for 521–680 CE, the temperature, precipitation and atmospheric circulation patterns are studied. The simulated cooling magnitude is then used as input for the growing degree day (GDD) model set-up for Southern Norway. This GDD model indicates the possible effects on agriculture for three different study areas in Southern Norway, representative of typical meteorological and landscape conditions. Pollen from bogs and archaeological records inside the study area are then analysed at high resolution (1–3 cm sample intervals) to give insights into the validity of the GDD model set-up with regard to the volcanic climate impact on the regional scale, and to link the different types of data sets. After the 536/540 CE double event, a maximum surface air cooling of up to 3.5 °C during the mean growing season is simulated regionally in Southern Norway. With a worst-case scenario cooling of 3 °C, the GDD model indicates crop failures were likely in our northernmost and western study areas, while crops were more likely to mature in the southeastern study area. These results are in agreement with the pollen records from the respective areas. During the sixth century, excavations show an abandonment of farms, severe social impact but also a continuation of occupation or a mix of those. In addition, archaeological findings from one of the excavation sites suggest wetter conditions for the mid-sixth century in Scandinavia, as simulated by individual ensemble members. Finally, we discuss the likely climate and societal impacts of the 536/540 CE volcanic double event by synthesising the new and available data sets for the whole Scandinavia.

The climate of the Northern Hemisphere (NH) in the mid-6th century was one of the coldest during the last 2 millennia based on multiple paleo-proxies. While the onset of this cold period can be clearly connected to the volcanic eruptions in 536 and 540 Common Era (CE), the duration, extent, and magnitude of the cold period are uncertain. Proxy data are sparse for the first millennium, which compounds the uncertainties of the reconstructions. To better understand the mechanisms of the prolonged cooling, we analyze new transient simulations over the Common Era and enhance the representation of mid-6th to 7th century climate by additional ensemble simulations covering 520–680 CE. We use the Max Planck Institute Earth System Model to apply the external forcing as recommended in the Paleoclimate Modelling Intercomparison Project phase 4. After the four large eruptions in 536, 540, 574, and 626 CE, a significant mean surface climate response in the NH lasting up to 20 years is simulated. The 2 m air temperature shows a cooling over the Arctic in winter, corresponding to the increase in Arctic sea ice, mainly in the Labrador Sea and to the east of Greenland. The increase in sea-ice extent relates to a decrease in the northward ocean heat transport into the Arctic within the first 2 years after the eruptions and to an increase in the Atlantic meridional overturning circulation, which peaks 10 years after the eruptions. A decrease in the global ocean heat content is simulated after the eruptions that does not recover during the simulation period. These ocean–sea-ice interactions sustain the surface cooling, as the cooling lasts longer than is expected solely from the direct effects of the volcanic forcing, and are thus responsible for the multi-decadal surface cooling. In boreal summer, the main cooling occurs over the continents at midlatitudes. A dipole pattern develops with high sea level pressure and a decrease in both precipitation and evaporation poleward of 40∘ N. In addition, more pronounced cooling over land compared to ocean leads to an enhanced land–sea contrast. While our model ensemble simulations show a similar ∼20-year summer cooling over NH land after the eruptions as tree ring reconstructions, a volcanic-induced century-long cooling, as reconstructed from tree ring data, does not occur in our simulations.

The mid-6th century is an outstanding period in climate history featuring one of the coldest decades in the past 2000 years. It was triggered by the 536/540 CE volcanic double event, creating the strongest decadal volcanic forcing in the last two millennia. The centuries of the first millennium are characterized by great societal changes, including the ending of antiquity and the beginning of early medieval state formations, a process believed to have been reinforced by the LALIA and the Justinian Plague. However, less is known about causal relationships between global cooling, regional climate, and local societal changes in Scandinavia after this volcanic double event. Here we aim to improve this understanding by combining global climate and local growing-degree-day (GDD) modeling for southern Norway.We use the PMIP4 past2k and the 6th-7th century (520-680 CE) MPI-ESM ensemble simulations, to analyze the atmospheric circulation and surface climate changes as a response to the 536/540 CE volcanic double event, focusing on Scandinavia. The ensemble mean reveals significant surface cooling up to 2K, accompanied by reduced precipitation up to 25% over Scandinavia during the growing season. However, single MPI-ESM model realizations show slight warming and increased precipitation reflecting different atmospheric circulation patterns over the years following the eruptions. Three sites are selected for the GDD model as a case study, representing different weather regimes in Southern Norway, which are then driven with the MPI-ESM ensemble data as input. The high-resolution data are compared to archaeological- and high-resolution pollen records, to shed more light on the climate, vegetation, and society impacts for southern Norway. We discuss the likely volcanic climate response over Scandinavia based on the model spread, atmospheric circulation change patterns, and the local archaeological and pollen records.

The early 19th century was the coldest period over the past 500 years, when strong tropical volcanic events and a solar minimum coincided. The 1809 unidentified eruption and the 1815 Tambora eruption happened consecutively during the Dalton minimum of solar irradiance; however, the relative role of the two forcing (volcano and solar) agents is still unclear. In this study, we examine the responses from a set of early 19th century simulations with combined and separated volcanic and solar forcing agents, as suggested in the protocol for the past1000 experiment of the Paleoclimate Modelling Intercomparison Project – Phase 4 (PMIP4). From 20-member ensemble simulations with the Max Planck Institute Earth system model (MPI-ESM1.2-LR), we find that the volcano- and solar-induced surface cooling is additive in the global mean/large scale, regardless of combining or separating the forcing agents. The two solar reconstructions (SATIRE (Spectral and Total Irradiance REconstruction-Millennia model) and PMOD (Physikalisch-Meteorologisches Observatorium Davos)) contribute to a cooling before and after 1815 of ∼0.05 and ∼0.15 K monthly average near-surface air cooling, respectively, indicating a limited solar contribution to the early 19th century cold period. The volcanic events provide the main cooling contributions, inducing a surface cooling that peaks at ∼0.82 K for the 1809 event and ∼1.35 K for Tambora. After the Tambora eruption, the temperature in most regions increases toward climatology largely within 5 years, along with the reduction of volcanic forcing. In the northern extratropical oceans, the temperature increases slowly at a constant rate until 1830, which is related to the reduction of seasonality and the concurrent changes in Arctic sea-ice extent. The albedo feedback of Arctic sea ice is found to be the main contributor to the Arctic amplification of the cooling signal. Several non-additive responses to solar and volcanic forcing happen on regional scales. In the atmosphere, the stratospheric polar vortex tends to strengthen when combining both volcano and solar forcing, even though the two forcing agents separately induce opposite-sign changes in stratospheric temperatures and zonal winds. In the ocean, when combining the two forcings, additional surface cold water propagates to the northern extratropics from the additional solar cooling in the tropics, which results in regional cooling along the propagation. Overall, this study not only quantifies the surface responses from combinations of the volcano and solar forcing, but also highlights the components that cannot be simply added from the responses of the individual forcing agents, indicating that a relatively small forcing agent (such as solar in early 19th century) can impact the response from the large forcing (such as the 1815 Tambora eruption) when considering regional climates.

In 1963 a series of eruptions of Mt. Agung, Indonesia, resulted in the third largest eruption of the 20th century and claimed about 1900 lives. Two eruptions of this series injected SO2 into the stratosphere, which can create a long-lasting stratospheric sulfate layer. The estimated mass flux of the first eruption was about twice as large as the mass flux of the second eruption. We followed the estimated emission profiles and assumed for the first eruption on 17 March an injection rate of 4.7 Tg SO2 and 2.3 Tg SO2 for the second eruption on 16 May. The injected sulfur forms a sulfate layer in the stratosphere. The evolution of sulfur is nonlinear and depends on the injection rate and aerosol background conditions. We performed ensembles of two model experiments, one with a single eruption and a second one with two eruptions. The two smaller eruptions result in a lower sulfur burden, smaller aerosol particles, and 0.1 to 0.3 Wm−2 (10 %–20 %) lower radiative forcing in monthly mean global average compared to the individual eruption experiment. The differences are the consequence of slightly stronger meridional transport due to different seasons of the eruptions, lower injection height of the second eruption, and the resulting different aerosol evolution. Overall, the evolution of the volcanic clouds is different in case of two eruptions than with a single eruption only. The differences between the two experiments are significant. We conclude that there is no justification to use one eruption only and both climatic eruptions should be taken into account in future emission datasets.

The climate in the Northern Hemisphere (NH) of the mid-6th century was one of the coldest during the last two millennia. The onset of this cold period is attributed to the volcanic double eruption event in 536 and 540 Common Era (CE) based on multiple paleo-proxies. Recently, there has been a debate about how long lasting and cold this volcanic induced cold period actually was. To better understand this, we analyze new transient simulations over the Common Era and enhance the representation of mid 6th to 7th century climate by additional ensemble simulations covering 520–680 CE. We use the Max Planck Institute Earth System Model and apply external forcing as recommended in the Paleo Model Intercomparison Project, Phase 4. After the four large eruptions in 536, 540, 574, and 626 CE, a significant surface climate response up to 20 years is simulated. The Northern Hemisphere 2 m air temperature, and precipitation decreases up to 2 K, and 0.2 mm day−1, respectively, and sea ice area increases up to 1.5 x 1012 m2. The global ocean heat content decreases drastically by 1.5 x 1023 Jm−1, which is significant for 30–40 years, and does not totally recover during the entire study period. The surface maps reveal atmospheric circulation changes with a hemispheric dipole pattern and land see contrast in the first two years after the eruptions. Poleward of ∼ 45° N higher sea level pressure and a decrease in hydrological variables occur, accompanied by a land see contrast, with decreased values over land and an increase in values over the ocean, which is especially pronounced for evaporation during boreal summer. During boreal winter, a positive North Atlantic Oscillation develops in the first year after (three out of the four) large eruptions. Analysing underlying mechanisms in the North Atlantic reveals that complex interaction between sea-ice expansion, changes in barotropic streamfunction and meridional overturning circulation leads to a reduction in the ocean heat transport, which then further enhances sea ice expansion impacting NH surface climate up to 20 years. Temperature records reconstructed from tree-rings in the NH agree well with the model simulations and show a similar ∼20 year cooling after the eruptions. A century of surface cooling starting in the mid-6th century, as shown from local tree-ring records from the Alps and Altai, does not occur in our volcanic climate model simulations, nor in the NH tree-ring compilation.

The Los Chocoyos (14.6°N, 91.2°W) supereruption happened ?75,000 years ago in Guatemala and was one of the largest eruptions of the past 100,000 years. It emitted enormous amounts of sulfur, chlorine, and bromine, with multi-decadal consequences for the global climate and environment. Here, we simulate the impact of a Los Chocoyos-like eruption on the quasi-biennial oscillation (QBO), an oscillation of zonal winds in the tropical stratosphere, with a comprehensive aerosol chemistry Earth System Model. We find a ?10-year disruption of the QBO starting 4 months post eruption, with anomalous easterly winds lasting ?5 years, followed by westerlies, before returning to QBO conditions with a slightly prolonged periodicity. Volcanic aerosol heating and ozone depletion cooling leads to the QBO disruption and anomalous wind regimes through radiative changes and wave-mean flow interactions. Different model ensembles, volcanic forcing scenarios and results of a second model back up the robustness of our results.

Large volcanic eruptions that reach the stratosphere cool the surface climate and impact the atmospheric circulation, feeding back on the local climate. The mid-6th century is an outstanding period in climate history that featured an extreme cold period, including one of the coldest decades in the past 2000 years. It was triggered by the 536/540 CE volcanic double event, creating the strongest decadal volcanic forcing in the last two millennia. During this period societal changes are recorded around the world, like the Great Migration period and the outbreak of the Justinian Plague. However, not a lot is known about the causal relationships between global cooling and societal change. Less is known also, about the impact of the large-scale atmospheric circulation on the regional climate, vegetation and society in Scandinavia after this volcanic double event. Here we aim to improve this understanding by combining global climate and regional growing-degree-day (GGD) modeling with climate proxies and archaeological records from Southeastern Norway.We use PMIP4 past2k runs and the MPI-ESM ensemble simulation of the 6th/7th century (520-680 CE), to analyze the atmospheric circulation, surface climate and vegetation changes as a response to the volcanic double event of 536/540 CE, over Scandinavia, specifically Southeastern Norway. Thereby we focus on the response of the major circulation patterns that influence the climate over Northern Europe: the positive and negative North Atlantic Oscillation, the Scandinavian blocking and the Atlantic ridge. The results of the GDD model, driven with the MPI-ESM model input, are compared to local pollen and climate records and archaeological data (e.g. grave density and settlement records) to shed more light on the local climate, vegetation and society impact. This comparison allows us to better understand how a natural hazard influenced local areas and climate records in Southeastern Norway. This study is part of the VIKINGS project, which focuses on the impact of volcanic eruptions on climate, environment and society in Norway/ Scandinavia.

Understanding how agricultural societies were impacted and adapted to past climate variations is critical to face to contemporary climate change and guaranty the food security (#SDG2 Zero Hunger). However, linking climate and change in the behaviour of a population are difficult to evidence. Here, we studied the climate variations of the period between 200 and 1300 CE and its impact on the pre-Viking and Viking societies in Southeastern Norway, including the adaptation and resilience of the agricultural management. This period includes, between 300 and 800 CE, one of the coldest period of the last 2000 years. We used a retrospective approach combining a multi-proxy analysis of lake sediments, including geochemical and palynological analyses, to reconstruct past changes in temperature and agricultural practices during the period 200-1300 CE. We associated variations in Ca/Ti ratio as a result of change in lake productivity with the temperature. The periods 200-300 and 800-1300 CE were warmer than the period between 300 and 800 CE, which is known as the “Dark Ages Cold Period” in the Northern Hemisphere. During this colder period, phases dominated by grazing activities (280-420 CE, 480-580 CE, 700-780 CE) alternated with phases dominated by the cultivation of cereals and hemp (before 280 CE, 420-480 CE, 580-700 CE, and after 800 CE). The alternation of these phases is synchronous of temperature changes. Cold periods are associated to livestock farming, and warmer periods to crop farming. This result suggests that when temperature no longer allowed crop farming, the food production specialized in animal breeding. The result of a Principal Component Analysis show a succession of phases of crisis, adaptation and resilience of the socio-environmental system. The Viking Age (800-1000 CE) started with an increase in temperature and corresponds to the warmest period between 200 and 1300 CE, allowing a larger development of the agriculture practices and society. Our results prove that the pre-Viking society adapted their agricultural practices to the climate variability of the Late Antiquity and that the Vikings expanded with climate warming.

Large explosive volcanic eruptions inject sulphur into the stratosphere where it is converted to sulphur dioxide and sulphate aerosols. Due to atmospheric circulation patterns, aerosols from high-latitude eruptions typically remain concentrated in the hemisphere in which they are injected. Eruptions in the high-latitude Northern Hemisphere could thus lead to a stronger hemispheric radiative forcing and surface climate response than tropical eruptions, a claim that is supported by a previous study based on proxy records and the coupled aerosol-general circulation model MAECHAM5-HAM. Additionally, the subsequent surface deposition of volcanic sulphate is potentially harmful to humans and ecosystems, and an improved understanding of the deposition over polar ice sheets can contribute to better reconstructions of historical volcanic forcing. On this basis, we model Icelandic explosive eruptions in a pre-industrial atmosphere, taking both volcanic sulphur and halogen loading into account. We use the fully coupled Earth system model CESM2 with the atmospheric component WACCM6, which extends to the lower thermosphere and has prognostic stratospheric aerosols and full chemistry. In order to study the volcanic impacts on the atmosphere, environment, and sulphate deposition, we vary eruption parameters such as sulphur and halogen loading, and injection altitude and season. The modelled volcanic sulphate deposition is compared to the deposition in ice cores following comparable historical eruptions. Furthermore, we evaluate the potential environmental impacts of sulphate deposition. To study inter-model differences, we also compare the CESM2-WACCM6 simulations to similar Icelandic eruption experiments simulated with MAECHAM5-HAM.

Major volcanic eruptions increase sulfate aerosols in the stratosphere. This causes a large-scale dimming effect with significant surface cooling and stratosphere warming. However, the climate impact differs for tropical and extratropical eruptions, and depends on the eruption season and height, and volcanic volatiles injections. In order to study different volcanic aerosol forcing and their climate impact, we perform simulations based on the fully coupled Community Earth System Model version 2 (CESM2) with the version 6 of the Whole Atmosphere Community Climate Model (WACCM6) with prognostic stratospheric aerosol and chemistry. In this study, explosive eruptions at 14.6 N and 63.6 N in January and July injecting 17 MT and 200 MT SO2 at 24 km with and without halogens are simulated, in line with Central American Volcanic Arc and Icelandic volcanic eruptions. Simulated changes in the stratospheric sulfate and halogen burdens, and related impacts on aerosol optical depth, radiation, ozone and surface climate are analyzed. These simulated volcanic eruption cases will be compared with simulations based on the aerosol-climate model MAECHAM5-HAM.

Extratropical volcanic eruptions are commonly thought to be less effective at driving large-scale surface cooling than tropical eruptions, and only the latter are commonly thought to be able to distribute sulfate globally. Here, we test both of these assumptions using a network of ice cores from the polar regions of Antarctica and Greenland covering the past 15’000 years and climate-aerosol modeling. We employ state-of-the-art analyses of trace elements, cryptoptephra and sulphur isotopes (Burke et al., 2019) to gain new insights into the timing of past eruptions, their stratospheric sulphur mass injections and subsequent sulphate aerosol lifecycle. We use this information to estimate the climate impact potential due to negative radiative forcing caused by Earth’s largest volcanic eruptions since the last Glacial. Our analysis encompasses over 1’000 eruptions and include the caldera-forming eruptions of Okmok II (Alaska, 43 BCE, VEI=6, 53°N; McConnell et al., 2020), Aniakchak II (Alaska, 1600s BCE, VEI=6, 57°N), Crater Lake (Mazama, Oregon, 5600s BCE, VEI=7, 43°N) and Laacher See (Germany, c. 13 ka BP, VEI=6, 50°N).We use our reconstructed radiative forcing and the coupled earth system models MPI-ESM1.2 and CESM (version 1.2.2) to analyze the climatic impact caused by these eruptions and compare the simulated temperature response with temperature reconstructions based on ultra-long tree-ring chronologies. Finally, based on these comparisons, we propose a number of stratigraphic age tie-points to anchor ice-core chronologies from Greenland (GICC05) and Antarctica (WD2014) to the absolute dated tree-ring chronology. We thereby aim to improve proxy synchronization throughout the Holocene -- a prerequisite for detection and attribution studies -- and invite the paleo-climate community to update climate proxy records based on ice cores to the latest chronologies. The European Research Council Grant 820047 under the European Union’s Horizon 2020 research and innovation program funded the research project THERA - Timing of Holocene Volcanic eruptions and their radiative aerosol forcing. References:Burke, A., Moore, K. A., Sigl, M., Nita, D. C., McConnell, J. R., and Adkins, J. F.: Stratospheric eruptions from tropical and extra-tropical volcanoes constrained using high-resolution sulfur isotopes in ice cores, Earth Planet Sc Lett, 521, 113-119, 2019.McConnell, J. R., Sigl, M., Plunkett, G., Burke, A., Kim, W., Raible, C. C., Wilson, A. I., Manning, J. G., Ludlow, F. M., Chellman, N. J., Innes, H. M., Yang, Z., Larsen, J. F., Schaefer, J. R., Kipfstuhl, S., Mojtabavi, S., Wilhelms, F., Opel, T., Meyer, H., and Steffensen, J. P.: Extreme climate after massive eruption of Alaska’s Okmok volcano in 43 BCE and effects on the late Roman Republic and Ptolemaic Kingdom, Proceedings of the National Academy of Sciences, 117, 15443-15449, 2020.

Uncovering anthropogenic and environmental drivers behind past biological change requires integrated analyses of long-term records from a diversity of disciplines. We applied an interdisciplinary approach exploring effects of human land-use and environmental changes on vegetation dynamics at Lake Ljøgottjern in southeastern Norway during the Holocene. Combined analysis of pollen and sedimentary ancient DNA (sedaDNA) metabarcoding of the sedimentary sequence of the lake describes the vegetation dynamics at different scales, and establishes a timeline for pastoral farming activities. We integrate this reconstruction with geochemical analysis of the sediments, climate data, archaeological evidence of local human settlement and regional human population dynamics. Our data covering the last 10,000 years reveals consistent vegetation signals from pollen and sedaDNA indicating periods of deforestation connected to cultivation, matching the archaeological evidence. Multivariate analysis integrating the environmental data from geochemical and archaeological reconstructions with the vegetation composition indicates that the vegetation dynamics at Lake Ljøgottjern were primarily related to natural processes from the base of the core (in ca. 8000 BCE, Mesolithic) up to the Early Iron Age (ca. 500 BCE–550 CE), when agricultural activities in the region intensified. The pollen signal reflects the establishment of a Bronze Age (ca. 1800–500 BCE) farm in the area, while subsequent intensification of pollen concentrations of cultivated plants combined with the first sedaDNA signals of cultivation and pastoralism are consistent with evidence of the establishment of farming closer to the lake at around 300 BCE. These signals also correspond to the intensification of agriculture in southeastern Norway in the first centuries of the Early Iron Age. Applying an interdisciplinary approach allows us to reconstruct anthropogenic and environmental dynamics, and untangle effects of human land-use and environmental changes on vegetation dynamics in southeastern Norway during the Holocene. publishedVersion

The supereruption of Los Chocoyos (14.6∘ N, 91.2∘ W) in Guatemala ∼84 kyr ago was one of the largest volcanic events of the past 100 000 years. Recent petrologic data show that the eruption released very large amounts of climate-relevant sulfur and ozone-destroying chlorine and bromine gases (523±94 Mt sulfur, 1200±156 Mt chlorine, and 2±0.46 Mt bromine). Using the Earth system model (ESM) of the Community Earth System Model version 2 (CESM2) coupled with the Whole Atmosphere Community Climate Model version 6 (WACCM6), we simulated the impacts of the sulfur- and halogen-rich Los Chocoyos eruption on the preindustrial Earth system. Our simulations show that elevated sulfate burden and aerosol optical depth (AOD) persists for 5 years in the model, while the volcanic halogens stay elevated for nearly 15 years. As a consequence, the eruption leads to a collapse of the ozone layer with global mean column ozone values dropping to 50 DU (80 % decrease) and leading to a 550 % increase in surface UV over the first 5 years, with potential impacts on the biosphere. The volcanic eruption shows an asymmetric-hemispheric response with enhanced aerosol, ozone, UV, and climate signals over the Northern Hemisphere. Surface climate is impacted globally due to peak AOD of >6, which leads to a maximum surface cooling of >6 K, precipitation and terrestrial net primary production decrease of >25 %, and sea ice area increases of 40 % in the first 3 years. Locally, a wetting (>100 %) and strong increase in net primary production (NPP) (>700 %) over northern Africa is simulated in the first 5 years and related to a southward shift of the Intertropical Convergence Zone (ITCZ) to the southern tropics. The ocean responds with pronounced El Niño conditions in the first 3 years that shift to the southern tropics and are coherent with the ITCZ change. Recovery to pre-eruption ozone levels and climate takes 15 years and 30 years, respectively. The long-lasting surface cooling is sustained by an immediate increase in the Arctic sea ice area, followed by a decrease in poleward ocean heat transport at 60∘ N which lasts up to 20 years. In contrast, when simulating Los Chocoyos conventionally by including sulfur and neglecting halogens, we simulate a larger sulfate burden and AOD, more pronounced surface climate changes, and an increase in column ozone. By comparing our aerosol chemistry ESM results to other supereruption simulations with aerosol climate models, we find a higher surface climate impact per injected sulfur amount than previous studies for our different sets of model experiments, since the CESM2(WACCM6) creates smaller aerosols with a longer lifetime, partly due to the interactive aerosol chemistry. As the model uncertainties for the climate response to supereruptions are very large, observational evidence from paleo archives and a coordinated model intercomparison would help to improve our understanding of the climate and environment response.

The mid of the 6th century is an outstanding period and started with an unusual cold period that lasted several years to decades, due to the 536/540 CE double eruption event, with the strongest decadal volcanic forcing in the last 2000 years. Evidence from multiple tree ring records from the Alps to the Altai Mountains in Russia identified a centennial cooling lasting from 536 up to 660 CE. A previous Earth System Model (ESM) study with reconstructed volcanic forcing covering 535-550 CE like conditions already found that the double eruption led to a global decrease in temperature and an increase in Arctic sea-ice for at least a decade. However, the simulations were too short to fully investigate the multi-decadal cooling event and the atmospheric forcing from this double volcanic eruption alone may not be enough to sustain such a prolonged cooling. To better understand forced versus internal decadal climate variability in the first millennium we have performed mid 6th century ensemble simulations with the MPI-ESM1.2 for the 520-680 CE period. The ensemble consists of 10 realizations, which were branched of the MPI-ESM1.2 PMIP4 Past2k run, including the evolv2k volcanic forcing.Here, we present results of this new set of the 6th-7th century MPI-ESM simulations in comparison to paleo-proxies. Summer surface temperatures are analyzed and compared with available tree-ring data, which fits very well for the entire 160 year period. As part of the VIKINGS project, special focus is placed on the impact of the 536/540 CE double volcanic eruption event on the surface climate in the Northern Hemisphere, in particular Scandinavia, Northern Europe and Siberia. The goal is to also compare the model data with new tree-ring and lake sediment proxies from southeastern Norway. Detailed comparison with proxy data will allow us to better understand the regional and seasonal climate variations of the 6th-7th century. Duration, strength and the possible mechanism for a long lasting volcanic induced cooling will be discussed.

Understanding how the Viking societies were impacted by past climate variability and how they adapted to it has hardly been investigated. Here, we have carried out a new multi-proxy investigation of lake sediments, including geochemical and palynological analyses, to reconstruct past changes in temperature and agricultural practices of pre-Viking and Viking societies in Southeastern Norway during the period between 200 and 1300 CE. The periods 200–300 and 800–1300 CE were warmer than the 300–800 CE period, which is known as the “Dark Ages Cold Period”. This cold period was punctuated by century-scale more temperate intervals, which were dominated by the cultivation of cereals and hemp (before 280 CE, 420–480 CE, 580–700 CE, and after 800 CE). In between, cold intervals were dominated by livestock farming. Our results demonstrate that the pre-Viking societies changed their agricultural strategy in response to climate variability during the Late Antiquity. publishedVersion

Uncertainty in the physicochemical and optical properties of volcanic ash particles creates errors in the detection and modeling of volcanic ash clouds and in quantification of their potential impacts. In this study, we provide a dataset that describes the physicochemical and optical properties of a representative selection of volcanic ash samples from nine different volcanic eruptions covering a wide range of silica contents (50 - 80 wt. % SiO2). We measured and calculated parameters describing the physical (size distribution, complex shape, and dense-rock equivalent mass density), chemical (bulk and surface composition) and optical (complex refractive index from ultra-violet to near-infrared wavelengths) properties of the volcanic ash and classified the samples according to their SiO2 and total alkali contents into the common igneous rock types Basalt to Rhyolite. We found that the mass density ranges between ρ = 2.49 and 2.98 g/cm3 for rhyolitic to basaltic ash types, and that the particle shape varies with changing particle size (d < 100 μm). The complex refractive indices in the wavelength range between λ = 300 nm and 1500 nm depends systematically on the composition of the samples. The real part values vary from n = 1.38 to 1.66 depending on ash type and wavelength and the imaginary part values from k = 0.00027 to 0.00268. We place our results into the context of existing data, and thus provide a comprehensive dataset that can be used for future and historic eruptions, when only basic information about the magma type producing the ash is known.

Halogenated very short-lived substances (VSLSs) are naturally produced in the ocean and emitted to the atmosphere. When transported to the stratosphere, these compounds can have a significant influence on the ozone layer and climate. During a research cruise on RV Sonne in the subtropical and tropical west Indian Ocean in July and August 2014, we measured the VSLSs, methyl iodide (CH3I) and for the first time bromoform (CHBr3) and dibromomethane (CH2Br2), in surface seawater and the marine atmosphere to derive their emission strengths. Using the Lagrangian particle dispersion model FLEXPART with ERA-Interim meteorological fields, we calculated the direct contribution of observed VSLS emissions to the stratospheric halogen burden during the Asian summer monsoon. Furthermore, we compare the in situ calculations with the interannual variability of transport from a larger area of the west Indian Ocean surface to the stratosphere for July 2000–2015. We found that the west Indian Ocean is a strong source for CHBr3 (910 pmol m−2 h−1), very strong source for CH2Br2 (930 pmol m−2 h−1), and an average source for CH3I (460 pmol m−2 h−1). The atmospheric transport from the tropical west Indian Ocean surface to the stratosphere experiences two main pathways. On very short timescales, especially relevant for the shortest-lived compound CH3I (3.5 days lifetime), convection above the Indian Ocean lifts oceanic air masses and VSLSs towards the tropopause. On a longer timescale, the Asian summer monsoon circulation transports oceanic VSLSs towards India and the Bay of Bengal, where they are lifted with the monsoon convection and reach stratospheric levels in the southeastern part of the Asian monsoon anticyclone. This transport pathway is more important for the longer-lived brominated compounds (17 and 150 days lifetime for CHBr3 and CH2Br2). The entrainment of CHBr3 and CH3I from the west Indian Ocean to the stratosphere during the Asian summer monsoon is lower than from previous cruises in the tropical west Pacific Ocean during boreal autumn and early winter but higher than from the tropical Atlantic during boreal summer. In contrast, the projected CH2Br2 entrainment was very high because of the high emissions during the west Indian Ocean cruise. The 16-year July time series shows highest interannual variability for the shortest-lived CH3I and lowest for the longest-lived CH2Br2. During this time period, a small increase in VSLS entrainment from the west Indian Ocean through the Asian monsoon to the stratosphere is found. Overall, this study confirms that the subtropical and tropical west Indian Ocean is an important source region of halogenated VSLSs, especially CH2Br2, to the troposphere and stratosphere during the Asian summer monsoon.

The super-eruption of Los Chocoyos, newly dated to 80.6 kyrs ago, in Guatemala was one of the largest volcanic events of the past 100 000 years. Recent petrologic data show that the eruption released very large amounts of climate-relevant sulfur and ozone destroying chlorine and bromine gases. Using the recently released Earth System Model CESM2(WACCM6) we simulate the impacts of the sulfur- and halogen-rich Los Chocoyos (~ 15° N) eruption on the pre-industrial Earth System for the eruption month January. Our model results show that enhanced modeled sulfate burden and aerosol optical depth (AOD) persists for five years, while the volcanic halogens stay elevated for nearly 15 years. As a consequence the eruption leads to a collapse of the ozone layer with global mean column ozone values dropping to 50 DU (80 % decrease) leading to a 550 % increase in surface UV over the first five years with potential impacts on the biosphere. The volcanic eruption shows an asymmetric hemispheric response with enhanced aerosol, ozone, UV, and climate signals over the Northern Hemisphere (NH). Surface climate is impacted globally due to peak AOD of > 6 leading to a maximum surface cooling of > 6 K, precipitation and terrestrial net primary production (NPP) decreases of > 25 %, and sea ice area increases of 40 % in the first three years. Locally, a wetting (> 100 %) and strong increase of NPP (> 700 %) over Northern Africa is simulated in the first five years related to a southwards shift of the Inter-Tropical Convergence Zone to the southern tropics. The ocean responds with El-Niño conditions in the first two years which are masked by the strong volcanic induced surface cooling. Recovery to pre-eruption ozone levels and climate takes 15 and 30 years respectively. The long lasting surface cooling is sustained by sea ice/ocean changes in the Arctic showing an immediate sea ice area increase followed by a decrease of poleward ocean heat transport at 60° N lasting up to 20 years. In contrast, when simulating Los Chocoyos conventionally, including sulfur and neglecting halogens, we simulate larger sulfate burden and AOD, more pronounced surface climate changes and an increase of column ozone. Comparing our aerosol chemistry ESM results to other super-eruption simulations with aerosol climate models we find a higher surface climate impact per injected sulfur amount than previous studies for our different sets of model experiments, since CESM2(WACCM6) creates smaller aerosols with a longer lifetime partly due to the interactive aerosol chemistry. As the model uncertainties for the climate response to super eruptions are very large observational evidence from paleo archives and a coordinated model intercomparison would help to improve our understanding of the climate and environment response.

The tropical tropopause layer (TTL) is the transition region between the well mixed, convective troposphere and the radiatively controlled stratosphere with air masses showing chemical and dynamical properties of both regions. The representation of the TTL in meteorological reanalysis data sets is important for studying the complex interactions of circulation, convection, trace gases, clouds and radiation. In this paper, we present the evaluation of TTL characteristics in reanalysis data sets that has been performed as part of the SPARC (Stratosphere– troposphere Processes and their Role in Climate) Reanalysis Intercomparison Project (S-RIP). The most recent atmospheric reanalysis data sets all provide realistic representations of the major characteristics of the temperature structure within the TTL. There is good agreement between reanalysis estimates of tropical mean temperatures and radio occultation data, with relatively small cold biases for most data sets. Temperatures at the cold point and lapse rate tropopause levels, on the other hand, show warm biases in reanalyses when compared to observations. This tropopause-level warm bias is related to the vertical resolution of the reanalysis data, with the smallest bias found for data sets with the highest vertical resolution around the tropopause. Differences of the cold point temperature maximise over equatorial Africa, related to Kelvin wave activity and associated disturbances in TTL temperatures. Model simulations of air mass transport into the stratosphere driven by reanalyses with a warm cold point bias can be expected to have too little dehydration. Interannual variability in reanalysis temperatures is best constrained in the upper TTL, with larger differences at levels below the cold point. The reanalyses reproduce the temperature responses to major dynamical and radiative signals such as volcanic eruptions and the QBO. Long-term reanalysis trends in temperature in the upper TTL show good agreement with trends derived from adjusted radiosonde data sets indicating significant stratospheric cooling of around −0.5 to −1 K/decade. At 100 hPa and the cold point, most of the reanalyses suggest small but significant cooling trends of −0.3 to −0.6 K/decade that are statistically consistent with trends based on the adjusted radiosonde data sets. Advances of the reanalysis and observational systems over the last decades have led to a clear improvement of the TTL reanalyses products over time. Biases of the temperature profiles and differences in interannual variability clearly decreased in 2006, when densely sampled radio occultation data started being assimilated by the reanalyses. While there is an overall good agreement, different reanalyses offer different advantages in the TTL such as realistic profile and cold point temperature, continuous time series or a realistic representation of signals of interannual variability. Their use in model simulations and in comparisons with climate model output should be tailored to their specific strengths and weaknesses.

Large explosive tropical volcanic eruptions inject high amounts of gases into the stratosphere, where they disperse globally through the large-scale meridional circulation. There is now increasing observational evidence that volcanic halogens can reach the upper troposphere and lower stratosphere. Here, we present the first study that combines measurement-based data of sulfur, chlorine and bromine releases from tropical volcanic eruptions with complex coupled chemistry climate model simulations taking radiative-dynamical-chemical feedbacks into account. Halogen model input parameters represent a size-time-region-wide average for the Central American eruptions over the last 200 ka ensuring a comprehensive perspective. The simulations reveal global, long-lasting impact on the ozone layer affecting atmospheric composition and circulation for a decade. Column ozone drops below 220 DU (ozone hole conditions) in the tropics, Arctic and Antarctica, increasing biologically active UV by 80 to 400%. Our model results could potentially be validated using high-resolution proxies from ice cores and pollen records.

We combine available observational data sets with Lagrangian atmospheric modelling in order to analyze the spatial and temporal variability of the CHBr3 injection into the stratosphere. Regional maxima with mixing ratios of up to 0.4–0.5 ppt at 17 km altitude are diagnosed to be over Central America (1) and over the Maritime Continent/West Pacific (2), both of which are confirmed by high-altitude aircraft campaigns. The CHBr3 maximum over Central America is caused by the co-occurrence of convectively-driven short transport time scales and strong regional sources, which in conjunction drive the seasonality of CHBr3 injection. Model results at a daily resolution reveal isolated, exceptionally high CHBr3 values in this region which are confirmed by measurements during the ACCENT campaign and do not occur in spatially or temporally averaged model fields. CHBr3 injection over the West Pacific is centered south of the equator due to strong oceanic sources underneath prescribed by the here applied bottom-up emission inventory. The globally strongest stratospheric CHBr3 injection of up to 0.6 ppt is diagnosed to occur over the region of India, Bay of Bengal and Arabian Sea (3), however, no data from aircraft campaigns are available to confirm this finding. Interannual variability of stratospheric CHBr3 injection of 10–20 % is to a large part driven by the variability of coupled ocean-atmosphere circulation systems. Long-term changes, on the other hand, correlate with the regional SST trends resulting in positive trends of stratospheric CHBr3 injection over the West Pacific and Asian monsoon region and negative trends over the East Pacific. For the tropical mean, these opposite regional trends balance each other out resulting in a relatively weak positive trend of 0.017 ± 0.012 ppt Br/dec for 1979–2013, corresponding 3 % Br/dec. The overall contribution of CHBr3 together with CH2Br2 to the stratospheric halogen loading accounts for 4.7 ppt Br, in good agreement with existing studies, with 50 %/50 % being injected in form of source and product gases, respectively.

Halogenated Very Short-lived Substances (VSLS), such as bromoform, dibromomethane and methyl iodide, are naturally produced in the oceans and are involved in ozone depletion in the troposphere and the stratosphere. The effect of climate change on the oceanic emissions of these compounds is not well quantified. Based on present-day observed global oceanic and atmospheric concentrations, and historic and future data from three CMIP5 models, past and future sea-to-air fluxes of these VSLS are calculated. The simulations are used to infer possible effects of projected changes of physical forcing on emissions in different oceanic regimes. CMIP5 model output for 1979–2100 from the historical scenario and the RCP scenarios 2.6 and 8.5 are used as input data for the emission calculations. Of the parameters that have the main influence on the sea-to-air fluxes, the global sea surface temperatures show a steady increase during the twenty-first century, while the projected changes of sea surface wind speed is very small. The calculated emissions based on the historical CMIP5 model runs (1979–2005) increased over the 26 year period and agree well with the emissions based on ERA-Interim data. The future sea-to-air fluxes of VSLS generally increase during the twenty-first century under the assumption of constant concentration fields in the ocean and atmosphere. The multi-model mean global emissions of bromoform increase by 29.4% (9.0%) between 1986 and 2005 and 2081–2100 under RCP 8.5 (2.6) and dibromomethane and methyl iodide emissions increase by 23.3% (6.4%) and 5.5% (1.5%), respectively. Uncertainties of the future emission estimates, driven by ongoing environmental changes such as changing oceanic productivity (not considered in this study) are discussed.

The current generation of Earth system models that participate in the Coupled Model Intercomparison Project phase 5 (CMIP5) does not, on average, produce a strengthened Northern Hemisphere (NH) polar vortex after large tropical volcanic eruptions as suggested by observational records. Here we investigate the impact of volcanic eruptions on the NH winter stratosphere with an ensemble of 20 model simulations of the Max Planck Institute Earth system model. We compare the dynamical impact in simulations of the very large 1815 Tambora eruption with the averaged dynamical response to the two largest eruptions of the CMIP5 historical simulations (the 1883 Krakatau and the 1991 Pinatubo eruptions). We find that for both the Tambora and the averaged Krakatau-Pinatubo eruptions the radiative perturbation only weakly affects the polar vortex directly. The position of the maximum temperature anomaly gradient is located at approximately 30°N, where we obtain significant westerly zonal wind anomalies between 10hPa and 30hPa. Under the very strong forcing of the Tambora eruption, the NH polar vortex is significantly strengthened because the subtropical westerly wind anomalies are sufficiently strong to robustly alter the propagation of planetary waves. The average response to the eruptions of Krakatau and Pinatubo reveals a slight strengthening of the polar vortex, but individual ensemble members differ substantially, indicating that internal variability plays a dominant role. For the Tambora eruption the ensemble variability of the zonal mean temperature and zonal wind anomalies during midwinter and late winter is significantly reduced compared to the volcanically unperturbed period.

Halogen- and sulfur-containing compounds are supersaturated in the surface ocean, which results in their emission to the atmosphere. These compounds can be transported to the stratosphere, where they impact ozone, the background aerosol layer, and climate. In this study we calculate the seasonal and interannual variability of transport from the West Indian Ocean (WIO) surface to the stratosphere for 2000–2016 with the Lagrangian transport model FLEXPART using ERA-Interim meteorological fields. We investigate the transport relevant for very short lived substances (VSLS) with tropospheric lifetimes corresponding to dimethylsulfide (1 day), methyl iodide (CH3I, 3.5 days), bromoform (CHBr3, 17 days), and dibromomethane (CH2Br2, 150 days). The stratospheric source gas injection of VSLS tracers from the WIO shows a distinct annual cycle associated with the Asian monsoon. Over the 16-year time series, a slight increase in source gas injection from the WIO to the stratosphere is found for all VSLS tracers and during all seasons. The interannual variability shows a relationship with sea surface temperatures in the WIO as well as the El Niño–Southern Oscillation. During boreal spring of El Niño, enhanced stratospheric injection of VSLS from the tropical WIO is caused by positive sea surface temperature anomalies and enhanced vertical uplift above the WIO. During boreal fall of La Niña, strong injection is related to enhanced atmospheric upward motion over the East Indian Ocean and a prolonged Indian summer monsoon season. Related physical mechanisms and uncertainties are discussed in this study. ©2018. American Geophysical Union. All Rights Reserved.

Highlights • Data set of Br and Cl emissions from 29 large CAVA eruptions (VEI > 5). • Melt inclusions are strongly enriched in chlorine and bromine compared to their respective matrix glasses. • Fluid partitioning is 4 to 68 times more efficient for Br than for Cl. • Subducted calcareous sediments are the major control on the arc-magmatic bromine contents. • Average CAVA eruption would add 368% EESC of recent annual loading to stratosphere. Abstract Large explosive volcanic eruptions inject gases, aerosols, and fine ashes into the stratosphere, potentially influencing climate and atmosphere composition on a global scale. Although the potential climate effect of chlorine (Cl) and bromine (Br) injections into the stratosphere is known, the global mass fluxes are poorly constrained. In this study we focus on the magmatic degassing systematics and budgets of Br and Cl, and on constraining the major sources of Br in a subduction setting. We therefore present a regional time series of Br and Cl emissions from 29 highly explosive eruptions throughout the Central American Volcanic Arc (CAVA), covering the last 200 ka, and a range of magmatic compositions and eruption magnitudes. We have measured Br and Cl in matrix glasses and melt inclusions using synchrotron radiation micro X-ray fluorescence spectrometry (SR micro-XRF) and electron microprobe, respectively. Melt inclusions of the CAVA tephras generally have higher Br (0.9 to 17.9 ppm) and Cl (770 to 3800 ppm) contents than the matrix glasses (0.39 to 1.5 ppm Br, 600 to 2800 ppm Cl). Moreover, the difference between maximum and minimum concentrations observed in melt inclusions of a given sample ranges between 9 and 90% of the maximum observed concentration for Br, and between 2 and 40% for Cl. Such intra-sample variations arise from variable pre-eruptive degassing of these halogens into a magmatic fluid phase. The relative loss of Br from the melt is 4 to 68 times higher than that of Cl. The masses of Br (2–1100 kt) and Cl (0.1 to 800 Mt) emitted by the eruptions generate instantaneous additions to the stratosphere potentially amounting to ∼6–5600% of the present-day stratospheric annual global loading of Equivalent Effective Stratospheric Chlorine. As the size of the stratospheric impact is primarily a function of eruption magnitude, we use magnitude-frequency relationships to estimate that eruptions adding ∼10% to resident EESC loading would occur every

Oceanic very short-lived substances (VSLSs), such as bromoform (CHBr3), contribute to stratospheric halogen loading and, thus, to ozone depletion. However, the amount, timing, and region of bromine delivery to the stratosphere through one of the main entrance gates, the Indian summer monsoon circulation, are still uncertain. In this study, we created two bromoform emission inventories with monthly resolution for the tropical Indian Ocean and west Pacific based on new in situ bromoform measurements and novel ocean biogeochemistry modeling. The mass transport and atmospheric mixing ratios of bromoform were modeled for the year 2014 with the particle dispersion model FLEXPART driven by ERA-Interim reanalysis. We compare results between two emission scenarios: (1) monthly averaged and (2) annually averaged emissions. Both simulations reproduce the atmospheric distribution of bromoform from ship- and aircraft-based observations in the boundary layer and upper troposphere above the Indian Ocean reasonably well. Using monthly resolved emissions, the main oceanic source regions for the stratosphere include the Arabian Sea and Bay of Bengal in boreal summer and the tropical west Pacific Ocean in boreal winter. The main stratospheric injection in boreal summer occurs over the southern tip of India associated with the high local oceanic sources and strong convection of the summer monsoon. In boreal winter more bromoform is entrained over the west Pacific than over the Indian Ocean. The annually averaged stratospheric injection of bromoform is in the same range whether using monthly averaged or annually averaged emissions in our Lagrangian calculations. However, monthly averaged emissions result in the highest mixing ratios within the Asian monsoon anticyclone in boreal summer and above the central Indian Ocean in boreal winter, while annually averaged emissions display a maximum above the west Indian Ocean in boreal spring. In the Asian summer monsoon anticyclone bromoform atmospheric mixing ratios vary by up to 50 % between using monthly averaged and annually averaged oceanic emissions. Our results underline that the seasonal and regional stratospheric bromine injection from the tropical Indian Ocean and west Pacific critically depend on the seasonality and spatial distribution of the VSLS emissions.

A suite of oxygenated volatile organic compounds (OVOCs – acetaldehyde, acetone, propanal, butanal and butanone) were measured concurrently in the surface water and atmosphere of the South China Sea and Sulu Sea in November 2011. A strong correlation was observed between all OVOC concentrations in the surface seawater along the entire cruise track, except for acetaldehyde, suggesting similar sources and sinks in the surface ocean. Additionally, several phytoplankton groups, such as haptophytes or pelagophytes, were also correlated to all OVOCs, indicating that phytoplankton may be an important source of marine OVOCs in the South China and Sulu seas. Humic- and protein-like fluorescent dissolved organic matter (FDOM) components seemed to be additional precursors for butanone and acetaldehyde. The measurement-inferred OVOC fluxes generally showed an uptake of atmospheric OVOCs by the ocean for all gases, except for butanal. A few important exceptions were found along the Borneo coast, where OVOC fluxes from the ocean to the atmosphere were inferred. The atmospheric OVOC mixing ratios over the northern coast of Borneo were relatively high compared with literature values, suggesting that this coastal region is a local hotspot for atmospheric OVOCs. The calculated amount of OVOCs entrained into the ocean seemed to be an important source of OVOCs to the surface ocean. When the fluxes were out of the ocean, marine OVOCs were found to be enough to control the locally measured OVOC distribution in the atmosphere. Based on our model calculations, at least 0.4 ppb of marine-derived acetone and butanone can reach the upper troposphere, where they may have an important influence on hydrogen oxide radical formation over the western Pacific Ocean.

Assessments of climate sensitivity to projected greenhouse gas concentrations underpin environmental policy decisions, with such assessments often based on model simulations of climate during recent centuries and millennia1, 2, 3. These simulations depend critically on accurate records of past aerosol forcing from global-scale volcanic eruptions, reconstructed from measurements of sulphate deposition in ice cores4, 5, 6. Non-uniform transport and deposition of volcanic fallout mean that multiple records from a wide array of ice cores must be combined to create accurate reconstructions. Here we re-evaluated the record of volcanic sulphate deposition using a much more extensive array of Antarctic ice cores. In our new reconstruction, many additional records have been added and dating of previously published records corrected through precise synchronization to the annually dated West Antarctic Ice Sheet Divide ice core7, improving and extending the record throughout the Common Era. Whereas agreement with existing reconstructions is excellent after 1500, we found a substantially different history of volcanic aerosol deposition before 1500; for example, global aerosol forcing values from some of the largest eruptions (for example, 1257 and 1458) previously were overestimated by 20–30% and others underestimated by 20–50%.

We investigate the contribution of oceanic methyl iodide (CH3I) to the stratospheric iodine budget. Based on CH3I measurements from three tropical ship campaigns and the Lagrangian transport model FLEXPART, we provide a detailed analysis of CH3I transport from the ocean surface to the cold point in the upper tropical tropopause layer (TTL). While average oceanic emissions differ by less than 50% from campaign to campaign, the measurements show much stronger variations within each campaign. A positive correlation between the oceanic CH3I emissions and the efficiency of CH3I troposphere–stratosphere transport has been identified for some cruise sections. The mechanism of strong horizontal surface winds triggering large emissions on the one hand and being associated with tropical convective systems, such as developing typhoons, on the other hand, could explain the identified correlations. As a result of the simultaneous occurrence of large CH3I emissions and strong vertical uplift, localized maximum mixing ratios of 0.6 ppt CH3I at the cold point have been determined for observed peak emissions during the SHIVA (Stratospheric Ozone: Halogen Impacts in a Varying Atmosphere)-Sonne research vessel campaign in the coastal western Pacific. The other two campaigns give considerably smaller maxima of 0.1 ppt CH3I in the open western Pacific and 0.03 ppt in the coastal eastern Atlantic. In order to assess the representativeness of the large local mixing ratios, we use climatological emission scenarios to derive global upper air estimates of CH3I abundances. The model results are compared with available upper air measurements, including data from the recent ATTREX and HIPPO2 aircraft campaigns. In the eastern Pacific region, the location of the available measurement campaigns in the upper TTL, the comparisons give a good agreement, indicating that around 0.01 to 0.02 ppt of CH3I enter the stratosphere. However, other tropical regions that are subject to stronger convective activity show larger CH3I entrainment, e.g., 0.08 ppt in the western Pacific. Overall our model results give a tropical contribution of 0.04 ppt CH3I to the stratospheric iodine budget. The strong variations in the geographical distribution of CH3I entrainment suggest that currently available upper air measurements are not representative of global estimates and further campaigns will be necessary in order to better understand the CH3I contribution to stratospheric iodine.

Sea surface and atmospheric measurements of dimethylsulphide (DMS) were performed during the TransBrom cruise in the western Pacific Ocean between Japan and Australia in October 2009. Air–sea DMS fluxes were computed between 0 and 30 μmol m−2 d−1, which are in agreement with those computed by the current climatology, and peak emissions of marine DMS into the atmosphere were found during the occurrence of tropical storm systems. Atmospheric variability in DMS, however, did not follow that of the computed fluxes and was more related to atmospheric transport processes. The computed emissions were used as input fields for the Lagrangian dispersion model FLEXPART, which was set up with actual meteorological fields from ERA-Interim data and different chemical lifetimes of DMS. A comparison with aircraft in situ data from the adjacent HIPPO2 campaign revealed an overall good agreement between modelled versus observed DMS profiles over the tropical western Pacific Ocean. Based on observed DMS emissions and meteorological fields along the cruise track, the model projected that up to 30 g S per month in the form of DMS, emitted from an area of 6 × 104 m2, can be transported above 17 km. This surprisingly large DMS entrainment into the stratosphere is disproportionate to the regional extent of the area of emissions and mainly due to the high convective activity in this region as simulated by the transport model. Thus, if DMS can cross the tropical tropopause layer (TTL), we suggest that the considerably larger area of the tropical western Pacific Ocean can be a source of sulphur to the stratosphere, which has not been considered as yet.

Reconstructions of the atmospheric sulfate aerosol burdens resulting from past volcanic eruptions are based on ice core-derived estimates of volcanic sulfate deposition and the assumption that the two quantities are directly proportional. We test this assumption within simulations of tropical volcanic stratospheric sulfur injections with the MAECHAM5-HAM aerosol-climate model. An ensemble of 70 simulations is analyzed, with SO2 injections ranging from 8.5 to 700 Tg, with eruptions in January and July. Modeled sulfate deposition flux to Antarctica shows excellent spatial correlation with ice core-derived estimates for Pinatubo and Tambora, although the comparison suggests the modeled flux to the ice sheets is 4–5 times too large. We find that Greenland and Antarctic deposition efficiencies (the ratio of sulfate flux to each ice sheet to the maximum hemispheric stratospheric sulfate aerosol burden) vary as a function of the magnitude and season of stratospheric sulfur injection. Changes in simulated sulfate deposition for large SO2 injections are connected to increases in aerosol particle size, which impact aerosol sedimentation velocity and radiative properties, the latter leading to strong dynamical changes including strengthening of the winter polar vortices, which inhibits the transport of stratospheric aerosols to high latitudes. The resulting relationship between Antarctic and Greenland volcanic sulfate deposition is nonlinear for very large eruptions, with significantly less sulfate deposition to Antarctica than to Greenland. These model results suggest that variability of deposition efficiency may be an important consideration in the interpretation of ice core sulfate signals for eruptions of Tambora-magnitude and larger.

We describe the main differences in simulations of stratospheric climate and variability by models within the fifth Coupled Model Intercomparison Project (CMIP5) that have a model top above the stratopause and relatively fine stratospheric vertical resolution (high-top), and those that have a model top below the stratopause (low-top). Although the simulation of mean stratospheric climate by the two model ensembles is similar, the low-top model ensemble has very weak stratospheric variability on daily and interannual time scales. The frequency of major sudden stratospheric warming events is strongly underestimated by the low-top models with less than half the frequency of events observed in the reanalysis data and high-top models. The lack of stratospheric variability in the low-top models affects their stratosphere-troposphere coupling, resulting in short-lived anomalies in the Northern Annular Mode, which do not produce long-lasting tropospheric impacts, as seen in observations. The lack of stratospheric variability, however, does not appear to have any impact on the ability of the low-top models to reproduce past stratospheric temperature trends. We find little improvement in the simulation of decadal variability for the high-top models compared to the low-top, which is likely related to the fact that neither ensemble produces a realistic dynamical response to volcanic eruptions.