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Marine phytoplankton are primary producers in ocean ecosystems and emit dimethyl sulfide (DMS) into the atmosphere. DMS emissions are the largest biological source of atmospheric sulfur and are one of the largest uncertainties in global climate modeling. DMS is oxidized to methanesulfonic acid (MSA), sulfur dioxide, and hydroperoxymethyl thioformate, all of which can be oxidized to sulfate. Ice core records of MSA are used to investigate past DMS emissions but rely on the implicit assumption that the relative yield of oxidation products from DMS remains constant. However, this assumption is uncertain because there are no long-term records that compare MSA to other DMS oxidation products. Here, we share the first long-term record of both MSA and DMS-derived biogenic sulfate concentration in Greenland ice core samples from 1200 to 2006 CE. While MSA declines on average by 0.2 µg S kg^–1over the industrial era, biogenic sulfate from DMS increases by 0.8 µg S kg^–1. This increasing biogenic sulfate contradicts previous assertions of declining North Atlantic primary productivity inferred from decreasing MSA concentrations in Greenland ice cores over the industrial era. The changing ratio of MSA to biogenic sulfate suggests that trends in MSA could be caused by time-varying atmospheric chemistry and that MSA concentrations alone should not be used to infer past primary productivity.

 

Anthropogenic sulfate aerosols are estimated to have offset 60% of greenhouse-gas-induced warming in the Arctic, a region warming four times faster than the rest of the world. However, sulfate radiative forcing estimates remain uncertain because the relative contributions from anthropogenic versus natural sources to total sulfate aerosols are unknown. Here we measure sulfur isotopes of sulfate in a Summit, Greenland ice core from 1850 to 2006 CE to quantify the contribution of anthropogenic sulfur emissions to ice core sulfate. We use a Keeling plot to determine the anthropogenic sulfur isotopic signature (δ³⁴S_anthro= +2.9 ± 0.3 ‰), and compare this result to a compilation of sulfur isotope measurements of oil and coal. Using δ³⁴S_anthro, we quantify anthropogenic sulfate concentration separated from natural sulfate. Anthropogenic sulfate concentration increases to 67 ± 7% of non-sea-salt sulfate (65.1 ± 20.2µg kg⁻¹) during peak anthropogenic emissions from 1960 to 1990 and decreases to 45 ± 11% of non-sea-salt sulfate (25.4 ± 12.8µg kg⁻¹) from 1996 to 2006. These observations provide the first long-term record of anthropogenic sulfate distinguished from natural sources (e.g. volcanoes, dimethyl sulfide), and can be used to evaluate model characterization of anthropogenic sulfate aerosol fraction and radiative forcing over the industrial era.

 

This dataset provides annual measurements of methanesulfonic acid (MSA) in Summit, Greenland ice core samples collected at variable resolution from 1200 to 2006. The abstract for the paper on these measurements is pasted below. The other measurements referenced in this abstract are published in Jongebloed et al. (2023) GRL, Jongebloed et al. (2023) ERL, and available in the Arctic Data Center (doi:10.18739/A26T0GX7K and doi:10.18739/A2N873162) Abstract: Marine phytoplankton are primary producers in ocean ecosystems and emit dimethyl sulfide (DMS) to the atmosphere. DMS emissions are the largest biological source of atmospheric sulfur and are one of the largest uncertainties in global climate modeling. DMS is oxidized to methanesulfonic acid (MSA), sulfur dioxide (SO2), and hydroperoxymethyl thioformate (HPMTF), all of which can be oxidized to sulfate. Ice core records of MSA are used to investigate past DMS emissions but rely on the implicit assumption that the relative yield of oxidation products from DMS remains constant. However, this assumption is uncertain because there are no long-term records that compare MSA to other DMS oxidation products. Here we share the first long-term record of both MSA and DMS-derived biogenic sulfate concentration in Greenland ice core samples from 1200 to 2006 CE. While MSA declines on average by 0.2 µg S kg-1 over the industrial era, biogenic sulfate from DMS increases by 0.8 µg S kg-1. This increasing biogenic sulfate contradicts previous assertions of declining North Atlantic primary productivity inferred from decreasing MSA concentrations in Greenland ice cores over the industrial era. The changing ratio of MSA to biogenic sulfate suggests that trends in MSA could be caused by time-varying atmospheric chemistry, and that MSA concentrations alone should not be used to infer past primary productivity. 

Anthropogenic sulfate aerosols are estimated to have offset sixty percent of greenhouse-gas-induced warming in the Arctic, a region warming four times faster than the rest of the world. However, sulfate radiative forcing estimates remain uncertain because the relative contributions from anthropogenic versus natural sources to total sulfate aerosols are unknown. Here we measure sulfur isotopes of sulfate in a Summit, Greenland ice core from 1850 to 2006 CE to quantify the contribution of anthropogenic sulfur emissions to ice core sulfate. We use a Keeling Plot to determine the anthropogenic sulfur isotopic signature (δ34Santhro = +2.9  0.3 ‰), and compare this result to a compilation of sulfur isotope measurements of oil and coal. Using δ34Santhro, we quantify anthropogenic sulfate concentration separated from natural sulfate. Anthropogenic sulfate concentration increases to 68 ± 7% of non-sea-salt sulfate (65.1 ± 20.2 µg kg-1) during peak anthropogenic emissions from 1960 to 1990 and decreases to 45 ± 11% of non-sea-salt sulfate (25.4 ± 12.8 µg kg-1) from 1996 to 2006. These observations provide the first long-term record of anthropogenic sulfate distinguished from natural sources (e.g., volcanoes, dimethyl sulfide), and can be used to evaluate model characterization of anthropogenic sulfate aerosol fraction and radiative forcing over the industrial era. These data include sulfur isotopes of sulfate measurements from a Greenland ice core from 1850-2006. The preindustrial dataset (1200-1850) is uploaded to the Arctic data center here: doi:10.18739/A2N873162 

Abstract. The injection of sulfur into the stratosphere by volcanic eruptions is thedominant driver of natural climate variability oninterannual to multidecadal timescales. Based on a set of continuous sulfateand sulfur records from a suite of ice cores from Greenland and Antarctica,the HolVol v.1.0 database includes estimates of the magnitudes andapproximate source latitudes of major volcanic stratospheric sulfurinjection (VSSI) events for the Holocene (from 9500 BCE or 11 500 years BP to1900 CE), constituting an extension of the previous record by 7000 years.The database incorporates new-generation ice-core aerosol records with asub-annual temporal resolution and a demonstrated sub-decadal dating accuracyand precision. By tightly aligning and stacking the ice-core records on theWD2014 chronology from Antarctica, we resolve long-standing inconsistenciesin the dating of ancient volcanic eruptions that arise from biased (i.e.,dated too old) ice-core chronologies over the Holocene for Greenland. Wereconstruct 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 bipolarsulfate 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 locationsis in agreement with prior reconstructions for the past 2500 years. Intotal, these eruptions injected 7410 Tg S into thestratosphere: 70 % from tropical eruptions and 25 % from NHextratropical eruptions. A long-term latitudinally and monthly resolvedstratospheric aerosol optical depth (SAOD) time series is reconstructed fromthe HolVol VSSI estimates, representing the first Holocene-scalereconstruction constrained by Greenland and Antarctica ice cores. These newlong-term reconstructions of past VSSI and SAOD variability confirm evidencefrom regional volcanic eruption chronologies (e.g., from Iceland) in showingthat the Early Holocene (9500–7000 BCE) experienced a higher number ofvolcanic eruptions (+16 %) and cumulative VSSI (+86 %) compared withthe past 2500 years. This increase coincides with the rapid retreat of icesheets during deglaciation, providing context for potential future increasesin volcanic activity in regions under projected glacier melting in the 21stcentury. The reconstructed VSSI and SAOD data are available at https://doi.org/10.1594/PANGAEA.928646 (Sigl et al., 2021). 

The Arctic is warming at almost four times the global rate. Cooling caused by anthropogenic aerosols has been estimated to offset sixty percent of greenhouse-gas-induced Arctic warming, but the contribution of aerosols to radiative forcing (RF) represents the largest uncertainty in estimating total RF, largely due to unknown preindustrial aerosol abundance. Here, sulfur isotope measurements in a Greenland ice core show that passive volcanic degassing contributes up to 66 ± 10% of preindustrial ice core sulfate in years without major eruptions. A state-of-the-art model indicates passive volcanic sulfur emissions influencing the Arctic are underestimated by up to a factor of three, possibly because many volcanic inventories do not include hydrogen sulfide emissions. Higher preindustrial volcanic sulfur emissions reduce modeled anthropogenic Arctic aerosol cooling by up to a factor of two (+0.11 to +0.29 W m-2 (watts per square meter)), suggesting that underestimating passive volcanic sulfur emissions has significant implications for anthropogenic-induced Arctic climate change. These data include sulfur isotopes of sulfate measurements from a Greenland ice core and volcanic gas measurements (CO2:S (carbon dioxide:sulfur) ratios) from various volcanoes and hot springs in Iceland. 

Abstract. The South Pole Ice Core (SPICEcore) was drilled in 2014–2016 to provide adetailed multi-proxy archive of paleoclimate conditions in East Antarcticaduring the Holocene and late Pleistocene. Interpretation of these recordsrequires an accurate depth–age relationship. Here, we present the SPICEcore (SP19) timescale for the age of the ice of SPICEcore. SP19 is synchronized to theWD2014 chronology from the West Antarctic Ice Sheet Divide (WAIS Divide) icecore using stratigraphic matching of 251 volcanic events. These eventsindicate an age of 54 302±519 BP (years before 1950) at thebottom of SPICEcore. Annual layers identified in sodium and magnesium ionsto 11 341 BP were used to interpolate between stratigraphic volcanic tiepoints, yielding an annually resolved chronology through the Holocene.Estimated timescale uncertainty during the Holocene is less than 18 yearsrelative to WD2014, with the exception of the interval between 1800 to 3100BP when uncertainty estimates reach ±25 years due to widely spacedvolcanic tie points. Prior to the Holocene, uncertainties remain within 124 years relative to WD2014. Results show an average Holocene accumulation rateof 7.4 cm yr−1 (water equivalent). The time variability of accumulation rateis consistent with expectations for steady-state ice flow through the modernspatial pattern of accumulation rate. Time variations in nitrateconcentration, nitrate seasonal amplitude and δ15N of N2 in turn are as expected for the accumulation rate variations. The highlyvariable yet well-constrained Holocene accumulation history at the site canhelp improve scientific understanding of deposition-sensitive climateproxies such as δ15N of N2 and photolyzed chemicalcompounds. 

A comprehensive record (WHV2020) of explosive volcanic eruptions in the last 11,000 years is reconstructed from the West Antarctica Ice Sheet Divide deep ice core (WDC). The chronological list of 426 large volcanic eruptions in the Southern Hemisphere and the low latitudes during the Holocene are of the highest quality of all volcanic records from ice cores, owing to the high‐resolution chemical measurement of the ice core and the exceptionally accurate WDC timescale. No apparent trend is found in the frequency (number of eruptions per millennium) of volcanic eruptions, and the number of eruptions in the most recent millennium (1,000–2,000 CE) is only slightly higher than the average in the last 11 millennia. The atmospheric aerosol mass loading of climate‐impacting sulfur, estimated from measured volcanic sulfate deposition, is dominated by explosive eruptions with extraordinarily high sulfur mass loading. Signals of three major volcanic eruptions are detected in the second half of the 17th century (1700–1600) BCE when the Thera volcano in the eastern Mediterranean was suspected to have erupted; the fact that these signals are synchronous with three volcanic eruptions detected in Greenland ice cores suggests that these are likely eruptions in the low latitudes and none should be attributed exclusively to Thera. A number of eruptions with very high sulfur mass loading took place shortly before and during an early Holocene climatic episode, the so‐called 8.2 ka event, and are speculated to have contributed to the initiation and magnitude of the cold event.

 

Variability in sea ice is a critical climate feedback, yet the seasonal behavior of Southern Hemisphere sea ice and climate across multiple timescales remains unclear. Here, we develop a seasonally resolved Holocene sea salt record using major ion measurements of the South Pole Ice Core (SPC14). We combine the SPC14 data with the GEOS‐Chem chemical transport model to demonstrate that the primary sea salt source switches seasonally from open water (summer) to sea ice (winter), with wintertime variations disproportionately responsible for the centennial to millennial scale structure in the record. We interpret increasing SPC14 and circum‐Antarctic Holocene sea salt concentrations, particularly between 8 and 10 ka, as reflecting a period of winter sea ice expansion. Between 5 and 6 ka, an anomalous drop in South Atlantic sector sea salt indicates a temporary sea ice reduction that may be coupled with Northern Hemisphere cooling and associated ocean circulation changes.