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© The Author(s), 2018. This article is distributed under the terms of the Creative Commons Attribution License. The definitive version was published in Journal of Geophysical Research: Oceans 123 (2018): 4853-4873, doi:10.1029/2018JC013888., The first full transarctic section of 228Ra in surface waters measured during GEOTRACES cruises PS94 and HLY1502 (2015) shows a consistent distribution with maximum activities in the transpolar drift. Activities in the central Arctic have increased from 2007 through 2011 to 2015. The increased 228Ra input is attributed to stronger wave action on shelves resulting from a longer ice‐free season. A concomitant decrease in the 228Th/228Ra ratio likely results from more rapid transit of surface waters depleted in 228Th by scavenging over the shelf. The 228Ra activities observed in intermediate waters (<1,500 m) in the Amundsen Basin are explained by ventilation with shelf water on a time scale of about 15–18 years, in good agreement with estimates based on SF6 and 129I/236U. The 228Th excess below the mixed layer up to 1,500 m depth can complement 234Th and 210Po as tracers of export production, after correction for the inherent excess resulting from the similarity of 228Ra and 228Th decay times. We show with a Th/Ra profile model that the 228Th/228Ra ratio below 1,500 m is inappropriate for this purpose because it is a delicate balance between horizontal supply of 228Ra and vertical flux of particulate 228Th. The accumulation of 226Ra in the deep Makarov Basin is not associated with an accumulation of Ba and can therefore be attributed to supply from decay of 230Th in the bottom sediment. We estimate a ventilation time of 480 years for the deep Makarov‐Canada Basin, in good agreement with previous estimates using other tracers., U.S. National Science Foundation Grant Numbers: OCE‐1458305, OCE‐1458424; US NSF Grant Number: OCE‐1433922

The rates of subsea permafrost degradation and occurrence of gas-migration pathways are key factors controlling the East Siberian Arctic Shelf (ESAS) methane (CH4) emissions, yet these factors still require assessment. It is thought that after inundation, permafrost-degradation rates would decrease over time and submerged thaw-lake taliks would freeze; therefore, no CH4 release would occur for millennia. Here we present results of the first comprehensive scientific re-drilling to show that subsea permafrost in the near-shore zone of the ESAS has a downward movement of the ice-bonded permafrost table of similar to 14 cm year(-1) over the past 31-32 years. Our data reveal polygonal thermokarst patterns on the seafloor and gas-migration associated with submerged taliks, ice scouring and pockmarks. Knowing the rate and mechanisms of subsea permafrost degradation is a prerequisite to meaningful predictions of near-future CH4 release in the Arctic.

It has been suggested that increasing terrestrial water discharge to the Arctic Ocean may partly occur as submarine groundwater discharge (SGD), yet there are no direct observations of this phenomenon in the Arctic shelf seas. This study tests the hypothesis that SGD does exist in the Siberian Arctic Shelf seas, but its dynamics may be largely controlled by complicated geocryological conditions such as permafrost. The field-observational approach in the southeastern Laptev Sea used a combination of hydrological (temperature, salinity), geological (bottom sediment drilling, geoelectric surveys), and geochemical (Ra-224, Ra-223, Ra-228, and Ra-226) techniques. Active SGD was documented in the vicinity of the Lena River delta with two different operational modes. In the first system, groundwater discharges through tectonogenic permafrost talik zones was registered in both winter and summer. The second SGD mechanism was cryogenic squeezing out of brine and water-soluble salts detected on the periphery of ice hummocks in the winter. The proposed mechanisms of groundwater transport and discharge in the Arctic land-shelf system is elaborated. Through salinity vs. Ra-224 and Ra-224/Ra-223 diagrams, the three main SGD-influenced water masses were identified and their end-member composition was constrained. Based on simple mass-balance box models, discharge rates at sites in the submarine permafrost talik zone were 1.7 x 10(6) m(3) d(-1) or 19.9 m(3) s(-1), which is much higher than the April discharge of the Yana River. Further studies should apply these techniques on a broader scale with the objective of elucidating the relative importance of the SGD transport vector relative to surface freshwater discharge for both water balance and aquatic components such as dissolved organic carbon, carbon dioxide, methane, and nutrients.

The Arctic Ocean is a small ocean basin surrounded by wide and shallow shelves receiving large river inputs. The radium quartet are four tracers of contact with sediments that give information on transport processes ranging in time scale from days to hundreds of years. 228Ra (5.8 y halflife) is a good tracer for surface water circulation. New 2015 GEOTRACES (sections GN01+GN04) 228Ra data show the first full Barents Sea to Bering Strait transect with maximum activities in the Transpolar Drift. We compare the 2015 section in the central Arctic with earlier Polarstern sections in 1987/1991, 2007 and 2011 and discuss reasons for increases in maximum 228Ra activities (Kipp et al., 2017). The penetration of 228Ra and its daughter 228Th to waters of intermediate depths (up to about 1500m) shows the exchange of these waters with shelf and slope sediments on the time scale of 228Ra decay. Input from the seafloor causes an enrichment of 228Ra and 226Ra in bottom waters. In deep waters (>2000m) of the Eurasian and Makarov basins 226Ra (1600 y halflife) accumulates to values around 16 dpm/100L or about twice the surface water concentration. It has been argued that export production increases with decreasing ice cover in the Arctic (Arrigo et al., 2008). Natural radionuclides can help to quantify export production rates, but the fluxes found may depend on the time scale of the tracer used. The most commonly used tracer 234Th/238U (24 d halflife) has a memory much shorter than a season. The 210Po/210Pb (138 d; Roca-Martí et al., 2016) and 228Th/228Ra ratios (1.9 y) are alternatives on a full seasonal time scale. Arrigo, K.R. et al., 2008. Geophys. Res. Lett. 35, L19603 Kipp, L. et al., 2017. ASLO 2017 OSM abstracts Roca-Martí, M. et al., 2016. Journal of Geophysical Research: Oceans 121, 5030-5049

It has been suggested that increasing freshwater discharge to the Arctic Ocean may also occur as submarine groundwater discharge (SGD), yet there are no direct observations of this phenomenon in the Arctic shelf seas. This study tests the hypothesis that SGD does exist in the Siberian-Arctic shelf seas but its dynamics may be largely controlled by complicated geocryological conditions such as permafrost. The field-observational approach in the southeast Laptev Sea used a combination of hydrological (temperature, salinity), geological (bottom sediment drilling, geoelectric surveys) and geochemical (224Ra, 223Ra and 222Rn) techniques. Active SGD was documented in the vicinity of the Lena River delta with two different operational modes. In the first system, groundwater discharges through tectonogenic permafrost talik zones was registered in both wintertime and summertime seasons. The second SGD mechanism was cryogenic squeezing out of brine and water-soluble salts detected on the periphery of ice hummocks in the wintertime season. The proposed mechanisms of groundwater transport and discharge in the arctic land-shelf system is elaborated. Through salinity versus 224Ra and 224Ra/223Ra diagrams, the three main SGD-influenced water masses were identified and their end-member composition was constrained. Further studies should apply these techniques to a broader scale with the objective to reach an estimate of the relative importance of the SGD transport vector relative to surface freshwater discharge for both the water balance and aquatic components such as dissolved organic carbon, carbon dioxide, methane, and nutrients.

Ocean acidification affects marine ecosystems and carbon cycling, and is considered a direct effect of anthropogenic carbon dioxide uptake from the atmosphere(1-3). Accumulation of atmospheric CO2 in ocean surface waters is predicted to make the ocean twice as acidic by the end of this century(4). The Arctic Ocean is particularly sensitive to ocean acidification because more CO2 can dissolve in cold water(5,6). Here we present observations of the chemical and physical characteristics of East Siberian Arctic Shelf waters from 1999,2000-2005,2008 and 2011, and find extreme aragonite undersaturation that reflects acidity levels in excess of those projected in this region for 2100. Dissolved inorganic carbon isotopic data and Markov chain Monte Carlo simulations of water sources using salinity and delta O-18 data suggest that the persistent acidification is driven by the degradation of terrestrial organic matter and discharge of Arctic river water with elevated CO2 concentrations, rather than by uptake of atmospheric CO2. We suggest that East Siberian Arctic Shelf waters may become more acidic if thawing permafrost leads to enhanced terrestrial organic carbon inputs and if freshwater additions continue to increase, which may affect their effciency as a source of CO2.

Thawing Arctic permafrost causes massive fluvial and erosional releases of dissolved and particulate organic carbon (DOC and POC) to coastal waters. Here we investigate how different sources and degradation of remobilized terrestrial carbon may affect large-scale carbon cycling, by comparing molecular and dual-isotope composition of waterborne high molecular weight DOC (>1kD, aka colloidal OC), POC, and sedimentary OC (SOC) across the East Siberian Arctic Shelves. Lignin phenol fingerprints demonstrate a longitudinal trend in relative contribution of terrestrial sources to coastal OC. Wax lipids and cutins were not detected in colloidal organic carbon (COC), in contrast to POC and SOC, suggesting that different terrestrial carbon pools partition into different aquatic carrier phases. The C-14 signal suggests overwhelmingly contemporary sources for COC, while POC and SOC are dominated by old C from Ice Complex Deposit (ICD) permafrost. Monte Carlo source apportionment (C-13, C-14) constrained that COC was dominated by terrestrial OC from topsoil permafrost (65%) and marine plankton (25%) with smaller contribution ICD and other older permafrost stocks (9%). This distribution is likely a result of inherent compositional matrix differences, possibly driven by organomineral associations. Modern OC found suspended in the surface water may be more exposed to degradation, in contrast to older OC that preferentially settles to the seafloor where it may be degraded on a longer timescale. The different sources which partition into DOC, POC, and SOC appear to have vastly different fates along the Eurasian Arctic coastal margin and may possibly respond on different timescales to climate change.

Sustained release of methane (CH4) to the atmosphere from thawing Arctic permafrost may be a positive and significant feedback to climate warming. Atmospheric venting of CH4 from the East Siberian Arctic Shelf (ESAS) was recently reported to be on par with flux from the Arctic tundra; however, the future scale of these releases remains unclear. Here, based on results of our latest observations, we show that CH4 emissions from this shelf are likely to be determined by the state of subsea permafrost degradation. We observed CH4 emissions from two previously understudied areas of the ESAS: the outer shelf, where subsea permafrost is predicted to be discontinuous or mostly degraded due to long submergence by seawater, and the near shore area, where deep/open taliks presumably form due to combined heating effects of seawater, river run-off, geothermal flux and pre-existing thermokarst. CH4 emissions from these areas emerge from largely thawed sediments via strong flare-like ebullition, producing fluxes that are orders of magnitude greater than fluxes observed in background areas underlain by largely frozen sediments. We suggest that progression of subsea permafrost thawing and decrease in ice extent could result in a significant increase in CH4 emissions from the ESAS.

The rapidly changing East Siberian Arctic Shelf (ESAS) receives large amounts of terrestrial organic carbon (OC) from coastal erosion and Russian-Arctic rivers. Climate warming increases thawing of coastal Ice Complex Deposits (ICD) and can change both the amount of released OC, as well as its propensity to be converted to greenhouse gases (fueling further global warming) or to be buried in coastal sediments. This study aimed to unravel the susceptibility to degradation, and transport and dispersal patterns of OC delivered to the ESAS. Bulk and molecular radiocarbon analyses on surface particulate matter (PM), sinking PM and underlying surface sediments illustrate the active release of old OC from coastal permafrost. Molecular tracers for recalcitrant soil OC showed ages of 3.4–13 14C-ky in surface PM and 5.5–18 14C-ky in surface sediments. The age difference of these markers between surface PM and surface sediments is larger (i) in regions with low OC accumulation rates, suggesting a weaker exchange between water column and sediments, and (ii) with increasing distance from the Lena River, suggesting preferential settling of fluvially derived old OC nearshore. A dual-carbon end-member mixing model showed that (i) contemporary terrestrial OC is dispersed mainly by horizontal transport while being subject to active degradation, (ii) marine OC is most affected by vertical transport and also actively degraded in the water column, and (iii) OC from ICD settles rapidly and dominates surface sediments. Preferential burial of ICD-OC released into ESAS coastal waters might therefore lower the suggested carbon cycle climate feedback from thawing ICD permafrost.

The rapidly changing East Siberian Arctic Shelf (ESAS) receives large amounts of terrestrial organic carbon (OC) from coastal erosion and Russian-Arctic rivers. Climate warming increases thawing of coastal Ice Complex Deposits (ICD) and can change both the amount of released OC, as well as its propensity to be converted to greenhouse gases (fueling further global warming) or to be buried in coastal sediments. This study aimed to unravel the susceptibility to degradation, and transport and dispersal patterns of OC delivered to the ESAS. Bulk and molecular radiocarbon analyses on surface particulate matter (PM), sinking PM and underlying surface sediments illustrate the active release of old OC from coastal permafrost. Molecular tracers for recalcitrant soil OC showed ages of 3.4–13 14C-ky in surface PM and 5.5–18 14C-ky in surface sediments. The age difference of these markers between surface PM and surface sediments is larger (i) in regions with low OC accumulation rates, suggesting a weaker exchange between water column and sediments, and (ii) with increasing distance from the Lena River, suggesting preferential settling of fluvially derived old OC nearshore. A dual-carbon end-member mixing model showed that (i) contemporary terrestrial OC is dispersed mainly by horizontal transport while being subject to active degradation, (ii) marine OC is most affected by vertical transport and also actively degraded in the water column, and (iii) OC from ICD settles rapidly and dominates surface sediments. Preferential burial of ICD-OC released into ESAS coastal waters might therefore lower the suggested carbon cycle climate feedback from thawing ICD permafrost.