Atmospheric iodine causes tropospheric ozone depletion and aerosol formation, both of which have significant climate impacts, and is an essential dietary element for humans. However, the evolution of atmospheric iodine levels at decadal and centennial scales is unknown. Here, we report iodine concentrations in the RECAP ice-core (coastal East Greenland) to investigate how atmospheric iodine levels in the North Atlantic have evolved over the past 260 years (1750–2011), this being the longest record of atmospheric iodine in the Northern Hemisphere. The levels of iodine tripled from 1950 to 2010. Our results suggest that this increase is driven by anthropogenic ozone pollution and enhanced sub-ice phytoplankton production associated with the recent thinning of Arctic sea ice. Increasing atmospheric iodine has accelerated ozone loss and has considerably enhanced iodine transport and deposition to the Northern Hemisphere continents. Future climate and anthropogenic forcing may continue to amplify oceanic iodine emissions with potentially significant health and environmental impacts at global scale.

Reconstructing the past variability of Arctic sea ice provides an essential context for recent multi-year sea ice decline, although few quantitative reconstructions cover the Holocene period prior to the earliest historical records 1,200 years ago. Photochemical recycling of bromine is observed over first-year, or seasonal, sea ice in so-called “bromine explosions” and we employ a 1-D chemistry transport model to quantify processes of bromine enrichment over first-year sea ice and depositional transport over multi-year sea ice and land ice. We report bromine enrichment in the Northwest Greenland Eemian NEEM ice core since the end of the Eemian interglacial 120,000 years ago, finding the maximum extension of first-year sea ice occurred approximately 9,000 years ago during the Holocene climate optimum, when Greenland temperatures were 2 to 3 °C above present values. First-year sea ice extent was lowest during the glacial stadials suggesting complete coverage of the Arctic Ocean by multi-year sea ice. These findings demonstrate a clear relationship between temperature and first-year sea ice extent in the Arctic and suggest multi-year sea ice will continue to decline as polar amplification drives Arctic temperatures beyond the 2 °C global average warming target of the recent COP21 Paris climate agreement.

Constraining the past sea ice variability in the Nordic Seas is critical for a comprehensive understanding of the abrupt Dansgaard-Oeschger (D-O) climate changes during the last glacial. Here we present unprecedentedly detailed sea ice proxy evidence from two Norwegian Sea sediment cores and an East Greenland ice core to resolve and constrain sea ice variations during four D-O events between 32 and 41 ka. Our independent sea ice records consistently reveal a millennial-scale variability and threshold response between an extensive seasonal sea ice cover in the Nordic Seas during cold stadials and reduced seasonal sea ice conditions during warmer interstadials. They document substantial and rapid sea ice reductions that may have happened within 250 y or less, concomitant with reinvigoration of deep convection in the Nordic Seas and the abrupt warming transitions in Greenland. Our empirical evidence thus underpins the cardinal role of rapid sea ice decline and related feedbacks to trigger abrupt and large-amplitude climate change of the glacial D-O events.

Abstract. The Law Dome site is ideal for the evaluation of sea ice proxies due to its location near to the Antarctic coast, regular and high accumulation throughout the year, an absence of surface melting or remobilization, and minimal multiyear sea ice. We present records of bromine and iodine concentrations and their enrichment beyond seawater compositions and compare these to satellite observations of first-year sea ice area in the 90–130° E sector of the Wilkes coast. Our findings support the results of previous studies of sea ice variability from Law Dome, indicating that Wilkes coast sea ice area is currently at its lowest level since the start of the 20th century. From the Law Dome DSS1213 firn core, 26 years of monthly deposition data indicate that the period of peak bromine enrichment is during austral spring–summer, from November to February. Results from a traverse along the lee (western) side of Law Dome show low levels of sodium and bromine deposition, with the greatest fluxes in the vicinity of the Law Dome summit. Finally, multidecadal variability in iodine enrichment appears well correlated to bromine enrichment, suggesting a common source of variability that may be related to the Interdecadal Pacific Oscillation (IPO).

Abstract. Although it has been demonstrated that the speed and magnitude of the recent Arctic sea ice decline is unprecedented for the past 1450 years, few records are available to provide a paleoclimate context for Arctic sea ice extent. Bromine enrichment in ice cores has been suggested to indicate the extent of newly formed sea ice areas. Despite the similarities among sea ice indicators and ice core bromine enrichment records, uncertainties still exist regarding the quantitative linkages between bromine reactive chemistry and the first-year sea ice surfaces. Here we present a 120 000-year record of bromine enrichment from the RECAP (REnland ice CAP) ice core, coastal east Greenland, and interpret it as a record of first-year sea ice. We compare it to existing sea ice records from marine cores and tentatively reconstruct past sea ice conditions in the North Atlantic as far north as the Fram Strait (50–85∘ N). Our interpretation implies that during the last deglaciation, the transition from multi-year to first-year sea ice started at ∼17.5 ka, synchronously with sea ice reductions observed in the eastern Nordic Seas and with the increase in North Atlantic ocean temperature. First-year sea ice reached its maximum at 12.4–11.8 ka during the Younger Dryas, after which open-water conditions started to dominate, consistent with sea ice records from the eastern Nordic Seas and the North Icelandic shelf. Our results show that over the last 120 000 years, multi-year sea ice extent was greatest during Marine Isotope Stage (MIS) 2 and possibly during MIS 4, with more extended first-year sea ice during MIS 3 and MIS 5. Sea ice extent during the Holocene (MIS 1) has been less than at any time in the last 120 000 years.

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Abstract. Atmospheric iodine chemistry has a large influence on oxidizing capacity and associated radiative impacts in the troposphere. However, information on the evolution of atmospheric iodine levels is restricted to the Industrial Period while its long-term natural variability remains unknown. The current levels of iodine in the atmosphere are controlled by anthropogenic ozone deposition to the ocean surface. Here, using high-resolution ice core measurements from coastal eastern Greenland (ReCAP ice core), we report the first record of atmospheric iodine variability during the Holocene (last 11,700 years). Surprisingly, our results reveal that the highest iodine concentrations in the record, found during the Holocene Thermal Maximum (~ 11,500-–5,500 years before -present). These high iodine levels could be driven by ocean primary productivity resulting in an Early Holocene “Biological Iodine Explosion”. The iodine trend during this past warm period is a useful observational constraint on projections of future changes in Arctic atmospheric composition and climate resulting from global warming.