skip to main content


This content will become publicly available on December 1, 2024

Title: The Marginal Ice Zone as a dominant source region of atmospheric mercury during central Arctic summertime
Abstract Atmospheric gaseous elemental mercury (GEM) concentrations in the Arctic exhibit a clear summertime maximum, while the origin of this peak is still a matter of debate in the community. Based on summertime observations during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition and a modeling approach, we further investigate the sources of atmospheric Hg in the central Arctic. Simulations with a generalized additive model (GAM) show that long-range transport of anthropogenic and terrestrial Hg from lower latitudes is a minor contribution (~2%), and more than 50% of the explained GEM variability is caused by oceanic evasion. A potential source contribution function (PSCF) analysis further shows that oceanic evasion is not significant throughout the ice-covered central Arctic Ocean but mainly occurs in the Marginal Ice Zone (MIZ) due to the specific environmental conditions in that region. Our results suggest that this regional process could be the leading contributor to the observed summertime GEM maximum. In the context of rapid Arctic warming and the observed increase in width of the MIZ, oceanic Hg evasion may become more significant and strengthen the role of the central Arctic Ocean as a summertime source of atmospheric Hg.  more » « less
Award ID(s):
1807163 1914781
NSF-PAR ID:
10465150
Author(s) / Creator(s):
; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; more » ; ; ; ; « less
Date Published:
Journal Name:
Nature Communications
Volume:
14
Issue:
1
ISSN:
2041-1723
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract

    The Bering Strait oceanic heat transport influences seasonal sea ice retreat and advance in the Chukchi Sea. Monitored since 1990, it depends on water temperature and factors controlling the volume transport, assumed to be local winds in the strait and an oceanic pressure difference between the Pacific and Arctic oceans (the “pressure head”). Recent work suggests that variability in the pressure head, especially during summer, relates to the strength of the zonal wind in the East Siberian Sea that raises or drops sea surface height in this area via Ekman transport. We confirm that westward winds in the East Siberian Sea relate to a broader central Arctic pattern of high sea level pressure and note that anticyclonic winds over the central Arctic Ocean also favor low September sea ice extent for the Arctic as a whole by promoting ice convergence and positive temperature anomalies. Month‐to‐month persistence in the volume transport and atmospheric circulation patterns is low, but the period 1980–2017 had a significant summertime (June–August) trend toward higher sea level pressure over the central Arctic Ocean, favoring increased transports. Some recent large heat transports are associated with high water temperatures, consistent with persistence of open water in the Chukchi Sea into winter and early ice retreat in spring. The highest heat transport recorded, October 2016, resulted from high water temperatures and ideal wind conditions yielding a record‐high volume transport. November and December 2005, the only months with southward volume (and thus heat) transports, were associated with southward winds in the strait.

     
    more » « less
  2. Abstract. Mercury (Hg) is emitted to the atmosphere mainly as volatile elemental Hg0. Oxidation to water-soluble HgII plays a major role in Hg deposition to ecosystems. Here, we implement a new mechanism for atmospheric Hg0HgII redox chemistry in the GEOS-Chem global model and examine the implications for the global atmospheric Hg budget and deposition patterns. Our simulation includes a new coupling of GEOS-Chem to an ocean general circulation model (MITgcm), enabling a global 3-D representation of atmosphere–ocean Hg0HgII cycling. We find that atomic bromine (Br) of marine organobromine origin is the main atmospheric Hg0 oxidant and that second-stage HgBr oxidation is mainly by the NO2 and HO2 radicals. The resulting chemical lifetime of tropospheric Hg0 against oxidation is 2.7 months, shorter than in previous models. Fast HgII atmospheric reduction must occur in order to match the  ∼ 6-month lifetime of Hg against deposition implied by the observed atmospheric variability of total gaseous mercury (TGM ≡ Hg0+HgII(g)). We implement this reduction in GEOS-Chem as photolysis of aqueous-phase HgII–organic complexes in aerosols and clouds, resulting in a TGM lifetime of 5.2 months against deposition and matching both mean observed TGM and its variability. Model sensitivity analysis shows that the interhemispheric gradient of TGM, previously used to infer a longer Hg lifetime against deposition, is misleading because Southern Hemisphere Hg mainly originates from oceanic emissions rather than transport from the Northern Hemisphere. The model reproduces the observed seasonal TGM variation at northern midlatitudes (maximum in February, minimum in September) driven by chemistry and oceanic evasion, but it does not reproduce the lack of seasonality observed at southern hemispheric marine sites. Aircraft observations in the lowermost stratosphere show a strong TGM–ozone relationship indicative of fast Hg0 oxidation, but we show that this relationship provides only a weak test of Hg chemistry because it is also influenced by mixing. The model reproduces observed Hg wet deposition fluxes over North America, Europe, and China with little bias (0–30%). It reproduces qualitatively the observed maximum in US deposition around the Gulf of Mexico, reflecting a combination of deep convection and availability of NO2 and HO2 radicals for second-stage HgBr oxidation. However, the magnitude of this maximum is underestimated. The relatively low observed Hg wet deposition over rural China is attributed to fast HgII reduction in the presence of high organic aerosol concentrations. We find that 80% of HgII deposition is to the global oceans, reflecting the marine origin of Br and low concentrations of organic aerosols for HgII reduction. Most of that deposition takes place to the tropical oceans due to the availability of HO2 and NO2 for second-stage HgBr oxidation.

     
    more » « less
  3. Abstract. The tundra plays a pivotal role in the Arctic mercury(Hg) cycle by storing atmospheric Hg deposition and shuttling it to theArctic Ocean. A recent study revealed that 70 % of the atmospheric Hgdeposition to the tundra occurs through gaseous elemental mercury (GEM or Hg(0))uptake by vegetation and soils. Processes controlling land–atmosphereexchange of Hg(0) in the Arctic tundra are central, but remainunderstudied. Here, we combine Hg stable isotope analysis of Hg(0) in theatmosphere, interstitial snow air, and soil pore air, with Hg(0) fluxmeasurements in a tundra ecosystem at Toolik Field Station in northernAlaska (USA). In the dark winter months, planetary boundary layer (PBL)conditions and Hg(0) concentrations were generally stable throughout the dayand small Hg(0) net deposition occurred. In spring, halogen-inducedatmospheric mercury depletion events (AMDEs) occurred, with the fastre-emission of Hg(0) after AMDEs resulting in net emission fluxes of Hg(0).During the short snow-free growing season in summer, vegetation uptake ofatmospheric Hg(0) enhanced atmospheric Hg(0) net deposition to the Arctictundra. At night, when PBL conditions were stable, ecosystem uptake ofatmospheric Hg(0) led to a depletion of atmospheric Hg(0). The night-timedecline of atmospheric Hg(0) was concomitant with a depletion of lighterHg(0) isotopes in the atmospheric Hg pool. The enrichment factor,ε202Hgvegetationuptake=-4.2 ‰ (±1.0 ‰) was consistentwith the preferential uptake of light Hg(0) isotopes by vegetation. Hg(0)flux measurements indicated a partial re-emission of Hg(0) during daytime,when solar radiation was strongest. Hg(0) concentrations in soil pore airwere depleted relative to atmospheric Hg(0) concentrations, concomitant withan enrichment of lighter Hg(0) isotopes in the soil pore air, ε202Hgsoilair-atmosphere=-1.00 ‰(±0.25 ‰) and E199Hgsoilair-atmosphere=0.07 ‰ (±0.04 ‰). Thesefirst Hg stable isotope measurements of Hg(0) in soil pore air areconsistent with the fractionation previously observed during Hg(0) oxidationby natural humic acids, suggesting abiotic oxidation as a cause for observedsoil Hg(0) uptake. The combination of Hg stable isotope fingerprints withHg(0) flux measurements and PBL stability assessment confirmed a dominantrole of Hg(0) uptake by vegetation in the terrestrial–atmosphere exchange ofHg(0) in the Arctic tundra. 
    more » « less
  4. null (Ed.)
    The marine-based West Antarctic Ice Sheet (WAIS) is currently locally retreating because of shifting wind-driven oceanic currents that transport warm waters toward the ice margin, resulting in ice shelf thinning and accelerated mass loss. Previous results from geologic drilling on Antarctica’s continental margins show significant variability in ice sheet extent during the late Neogene and Quaternary. Climate and ice sheet models indicate a fundamental role for oceanic heat in controlling ice sheet variability over at least the past 20 My. Although evidence for past ice sheet variability is available from ice-proximal marine settings, sedimentary sequences from the continental shelf and rise are required to evaluate the extent of past ice sheet variability and the associated forcings and feedbacks. International Ocean Discovery Program Expedition 374 drilled a latitudinal and depth transect of five sites from the outer continental shelf to rise in the central Ross Sea to resolve Neogene and Quaternary relationships between climatic and oceanic change and WAIS evolution. The Ross Sea was targeted because numerical ice sheet models indicate that this sector of Antarctica responds sensitively to changes in ocean heat flux. Expedition 374 was designed for optimal data-model integration to enable an improved understanding of Antarctic Ice Sheet (AIS) mass balance during warmer-than-present climates (e.g., the Pleistocene “super interglacials,” the mid-Pliocene, and the Miocene Climatic Optimum). The principal goals of Expedition 374 were to: 1. Evaluate the contribution of West Antarctica to far-field ice volume and sea level estimates; 2. Reconstruct ice-proximal oceanic and atmospheric temperatures to quantify past polar amplification; 3. Assess the role of oceanic forcing (e.g., temperature and sea level) on AIS variability; 4. Identify the sensitivity of the AIS to Earth’s orbital configuration under a variety of climate boundary conditions; and 5. Reconstruct Ross Sea paleobathymetry to examine relationships between seafloor geometry, ice sheet variability, and global climate. To achieve these objectives, postcruise studies will: 1. Use data and models to reconcile intervals of maximum Neogene and Quaternary ice advance and retreat with far-field records of eustatic sea level; 2. Reconstruct past changes in oceanic and atmospheric temperatures using a multiproxy approach; 3. Reconstruct Neogene and Quaternary sea ice margin fluctuations and correlate these records to existing inner continental shelf records; 4. Examine relationships among WAIS variability, Earth’s orbital configuration, oceanic temperature and circulation, and atmospheric pCO2; and 5. Constrain the timing of Ross Sea continental shelf overdeepening and assess its impact on Neogene and Quaternary ice dynamics. Expedition 374 departed from Lyttelton, New Zealand, in January 2018 and returned in March 2018. We recovered 1292.70 m of high-quality core from five sites spanning the early Miocene to late Quaternary. Three sites were cored on the continental shelf (Sites U1521, U1522, and U1523). At Site U1521, we cored a 650 m thick sequence of interbedded diamictite and diatom-rich mudstone penetrating seismic Ross Sea Unconformity 4 (RSU4). The depositional reconstructions of past glacial and open-marine conditions at this site will provide unprecedented insight into environmental change on the Antarctic continental shelf during the late early and middle Miocene. At Site U1522, we cored a discontinuous late Miocene to Pleistocene sequence of glacial and glaciomarine strata from the outer shelf with the primary objective of penetrating and dating RSU3, which is interpreted to reflect the first continental shelf–wide expansion of East and West Antarctic ice streams. Site U1523, located on the outer continental shelf, targeted a sediment drift beneath the westward-flowing Antarctic Slope Current (ASC) to test the hypothesis that changes in ASC vigor regulate ocean heat flux onto the continental shelf and thus ice sheet mass balance. We also cored two sites on the continental rise and slope. At Site U1524, we recovered a Plio–Pleistocene sedimentary sequence from the levee of the Hillary Canyon, one of the largest conduits of Antarctic Bottom Water from the continental shelf to the abyssal ocean. Site U1524 was designed to penetrate into middle Miocene and older strata, but coring was initially interrupted by drifting sea ice that forced us to abandon coring in Hole U1524A at 399.5 m drilling depth below seafloor (DSF). We moved to a nearby alternate site on the continental slope (Site U1525) to core a single hole designed to complement the record at Site U1524. We returned to Site U1524 after the sea ice cleared and cored Hole U1524C with the rotary core barrel system with the intention of reaching the target depth of 1000 m DSF. However, we were forced to terminate Hole U1524C at 441.9 m DSF because of a mechanical failure with the vessel that resulted in termination of all drilling operations and forced us to return to Lyttelton 16 days earlier than scheduled. The loss of 39% of our operational days significantly impacted our ability to achieve all Expedition 374 objectives. In particular, we were not able to recover continuous middle Miocene sequences from the continental rise designed to complement the discontinuous record from continental shelf Site U1521. The mechanical failure also meant we could not recover cores from proposed Site RSCR-19A, which was targeted to obtain a high-fidelity, continuous record of upper Neogene and Quaternary pelagic/hemipelagic sedimentation. Despite our failure to recover a continental shelf-to-rise Miocene transect, records from Sites U1522, U1524, and U1525 and legacy cores from the Antarctic Geological Drilling Project (ANDRILL) can be integrated to develop a shelf-to-rise Plio–Pleistocene transect. 
    more » « less
  5. Abstract

    Arctic surface warming under greenhouse gas forcing peaks in winter and reaches its minimum during summer in both observations and model projections. Many mechanisms have been proposed to explain this seasonal asymmetry, but disentangling these processes remains a challenge in the interpretation of general circulation model (GCM) experiments. To isolate these mechanisms, we use an idealized single-column sea ice model (SCM) that captures the seasonal pattern of Arctic warming. SCM experiments demonstrate that as sea ice melts and exposes open ocean, the accompanying increase in effective surface heat capacity alone can produce the observed pattern of peak warming in early winter (shifting to late winter under increased forcing) by slowing the seasonal heating rate, thus delaying the phase and reducing the amplitude of the seasonal cycle of surface temperature. To investigate warming seasonality in more complex models, we perform GCM experiments that individually isolate sea ice albedo and thermodynamic effects under CO2forcing. These also show a key role for the effective heat capacity of sea ice in promoting seasonal asymmetry through suppressing summer warming, in addition to precluding summer climatological inversions and a positive summer lapse-rate feedback. Peak winter warming in GCM experiments is further supported by a positive winter lapse-rate feedback, due to cold initial surface temperatures and strong surface-trapped warming that are enabled by the albedo effects of sea ice alone. While many factors contribute to the seasonal pattern of Arctic warming, these results highlight changes in effective surface heat capacity as a central mechanism supporting this seasonality.

    Significance Statement

    Under increasing concentrations of atmospheric greenhouse gases, the strongest Arctic warming has occurred during early winter, but the reasons for this seasonal pattern of warming are not well understood. We use experiments in both simple and complex models with certain sea ice processes turned on and off to disentangle potential drivers of seasonality in Arctic warming. When sea ice melts and open ocean is exposed, surface temperatures are slower to reach the warm-season maximum and slower to cool back down below freezing in early winter. We find that this process alone can produce the observed pattern of maximum Arctic warming in early winter, highlighting a fundamental mechanism for the seasonality of Arctic warming.

     
    more » « less