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Ice core measurements reveal dipole-like snow accumulation trends over West Antarctica throughout the 20th century, with an increase of >2000 billion metric tons over the Antarctic Peninsula and Ellsworth Land but a decrease of ~500 billion metric tons over Marie Byrd Land. Although atmospheric teleconnections were frequently revealed, linking variability between tropics and higher latitudes on interannual and decadal timescales, centennial-scale teleconnection is absent from literature. Here, using statistical analysis and numerical experiments, we reveal that changes of tropical oceans throughout the 20th century drive the long-term Antarctic snowfall trend. A pronounced warming over the tropical Atlantic and a moderate cooling over the equatorial Pacific have driven an adjustment of moisture transport and thus snowfall pattern in West Antarctica. Our study reveals a centennial tropical-polar teleconnection, producing long-term trends with opposing changes across the regions. Remote forcing from the tropics increased the mass accumulation over Antarctica, balanced rapid iceshelf thinning in recent decades, contributing to global sea-level changes. 

Abstract. Comprehensive evaluation of the effects of post-depositional processing is a prerequisite for appropriately interpreting ice-core records of nitrate concentration and isotopes. In this study, we developed an inverse model that uses archived snow/ice-core nitrate signals to reconstruct primary nitrate flux (i.e., the deposition flux of nitrate to surface snow that originates from long-range transport or stratospheric input) and its isotopes (δ15N and Δ17O). The model was then applied to two polar sites, Summit, Greenland, and Dome C, Antarctica, using measured snowpack nitrate concentration and isotope profiles in the top few meters. At Summit, the model successfully reproduced the observed atmospheric δ15N(NO3-) and Δ17O(NO3-) and their seasonality. The model was also able to reasonably reproduce the observed snowpack nitrate profiles at Dome C as well as the skin layer and atmospheric δ15N(NO3-) and Δ17O(NO3-) at the annual scale. The calculated Fpri at Summit was 6.9 × 10−6 kgN m2 a−1, and the calculated Δ17O(NO3-) of Fpri is consistent with atmospheric observations in the Northern Hemisphere. However, the calculated δ15N(NO3-) of Fpri displays an opposite seasonal pattern to atmospheric observations in the northern mid-latitudes, but it is consistent with observations in two Arctic coastal sites. The calculated Fpri at Dome C varies from 1.5 to 2.2 × 10−6 kgN m−2 a−1, with δ15N(NO3-) of Fpri varying from 6.2 ‰ to 29.3 ‰ and Δ17O(NO3-) of Fpri varying from 48.8 ‰ to 52.6 ‰. The calculated Fpri at Dome C is close to the previous estimated stratospheric denitrification flux in Antarctica, and the high δ15N(NO3-) and Δ17O(NO3-) of Fpri at Dome C also point towards the dominant role of stratospheric origin of primary nitrate to Dome C. 

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 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 

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. Discerning mechanisms of sulfate formation during fine-particle pollution (referred to as haze hereafter) in Beijing is important for understanding the rapid evolution of haze and for developing cost-effective air pollution mitigation strategies. Here we present observations of the oxygen-17 excess of PM_2.5 sulfate (Δ¹⁷O(SO₄²⁻)) collected in Beijing haze from October 2014 to January 2015 to constrain possible sulfate formation pathways. Throughout the sampling campaign, the 12-hourly averaged PM_2.5 concentrations ranged from 16 to 323µg m⁻³ with a mean of (141  ±  88 (1σ))µg m⁻³, with SO₄²⁻ representing 8–25% of PM_2.5 mass. The observed Δ¹⁷O(SO₄²⁻) varied from 0.1 to 1.6‰ with a mean of (0.9  ±  0.3)‰. Δ¹⁷O(SO₄²⁻) increased with PM_2.5 levels in October 2014 while the opposite trend was observed from November 2014 to January 2015. Our estimate suggested that in-cloud reactions dominated sulfate production on polluted days (PDs, PM_2.5  ≥  75µg m⁻³) of Case II in October 2014 due to the relatively high cloud liquid water content, with a fractional contribution of up to 68%. During PDs of Cases I and III–V, heterogeneous sulfate production (P_het) was estimated to contribute 41–54% to total sulfate formation with a mean of (48  ±  5)%. For the specific mechanisms of heterogeneous oxidation of SO₂, chemical reaction kinetics calculations suggested S(IV) ( = SO₂ ⚫H₂O+HSO₃⁻  +  SO₃²⁻) oxidation by H₂O₂ in aerosol water accounted for 5–13% of P_het. The relative importance of heterogeneous sulfate production by other mechanisms was constrained by our observed Δ¹⁷O(SO₄²⁻). Heterogeneous sulfate production via S(IV) oxidation by O₃ was estimated to contribute 21–22% of P_het on average. Heterogeneous sulfate production pathways that result in zero-Δ¹⁷O(SO₄²⁻), such as S(IV) oxidation by NO₂ in aerosol water and/or by O₂ via a radical chain mechanism, contributed the remaining 66–73% of P_het. The assumption about the thermodynamic state of aerosols (stable or metastable) was found to significantly influence the calculated aerosol pH (7.6  ±  0.1 or 4.7  ±  1.1, respectively), and thus influence the relative importance of heterogeneous sulfate production via S(IV) oxidation by NO₂ and by O₂. Our local atmospheric conditions-based calculations suggest sulfate formation via NO₂ oxidation can be the dominant pathway in aerosols at high-pH conditions calculated assuming stable state while S(IV) oxidation by O₂ can be the dominant pathway providing that highly acidic aerosols (pH ≤ 3) exist. Our local atmospheric-conditions-based calculations illustrate the utility of Δ¹⁷O(SO₄²⁻) for quantifying sulfate formation pathways, but this estimate may be further improved with future regional modeling work.