Sulfate and nitrate firn concentrations on the Greenland ice sheet

Intercomparison of three new chemical ice core records from northern Greenland (covering the time span from approximately 1500 A.D. to present) with previously published records for southern and central Greenland reveals a uniform timing of anthropogenic changes in sulfate and nitrate firn concentrations over the entire ice sheet. The anthropogenic sulfate increase started around 1890, was interrupted by a transient decrease in the 1930s, and has resumed a major increase since 1950. Since the late 1970s though, a significant 30% decline in Greenland sulfate firn levels can be documented. The maximum anthropogenic increase in northern Greenland sulfate firn concentrations (up to 200-230 ppb) is 2-3 times larger than in southern and central Greenland. Nitrate records show an essentially steady increase since 1950 and, documented for the first time, a slight reduction during most recent years. Maximum nitrate firn levels of 100-130 ppb exceed the preindustrial background by 100% all over the Greenland ice sheet. Comparison with anthropogenic SO2 and NO x emission records indicates that the major increase in sulfate firn concentrations since 1950 can be attributed to Eurasian sources, while firn levels during the first half of this century appear to be dominated by North American emissions. A stronger North American source contribution is indicated over the entire 20th century in the case of nitrate. Applying a macroscopic deposition model separate time series for wet and dry deposition were derived which revealed a close correspondence of wet deposited sulfate with the timing of U.S. emissions, while the temporal evolution of Eurasian emissions is mainly reflected in the dry sulfate deposition record. During this century wet sulfate deposition increased by a factor of two while the total dry sulfate deposition flux increased by more than 500%. Wet and dry nitrate deposition both increased by 100% during the same period.

(Table 1) Characteristics of marine snow and ice samples at Barrow, Alaska

We measured light absorption in 42 marine snow, sea ice, seawater, brine, and frost flower samples collected during the OASIS field campaign between February 27 and April 15, 2009. Samples represented multiple sites between landfast ice and open pack ice in coastal areas approximately 5 km west of Barrow, Alaska. The chromophores that are most commonly measured in snow, H2O2, NO3-, and NO2-, on average account for less than 1% of sunlight absorption in our samples. Instead, light absorption is dominated by unidentified "residual" species, likely organic compounds. Light absorption coefficients for the frost flowers on first-year sea ice are, on average, 40 times larger than values for terrestrial snow samples at Barrow, suggesting very large rates of photochemical reactions in frost flowers. For our marine samples the calculated rates of sunlight absorption and OH production from known chromophores are (0.1-1.4) x 10**14 (photons/cm**3/s) and (5-70) x 10**-12 (mol/L/s), respectively. Our residual spectra are similar to spectra of marine chromophoric dissolved organic matter (CDOM), suggesting that CDOM is the dominant chromophore in our samples. Based on our light absorption measurements we estimate dissolved organic carbon (DOC) concentrations in Barrow seawater and frost flowers as approximately 130 and 360 µM C, respectively. We expect that CDOM is a major source of OH in our marine samples, and it is likely to have other significant photochemistry as well.

Mercury content and isotopic composition of frost flower, surface snow and brine samples near Barrow, Alaska

Frost flowers are ice crystals that grow on refreezing sea ice leads in Polar Regions by wicking brine from the sea ice surface and accumulating vapor phase condensate. These crystals contain high concentrations of mercury (Hg) and are believed to be a source of reactive halogens, but their role in Hg cycling and impact on the fate of Hg deposited during atmospheric mercury depletion events (AMDEs) are not well understood. We collected frost flowers growing on refreezing sea ice near Barrow, Alaska (U.S.A.) during an AMDE in March 2009 and measured Hg concentrations and Hg stable isotope ratios in these samples to determine the origin of Hg associated with the crystals. We observed decreasing Delta199Hg values in the crystals as they grew from new wet frost flowers (mean Delta199Hg = 0.77 ± 0.13 per mil, 1 s.d.) to older dry frost flowers (mean Delta199Hg = 0.10 ± 0.05 per mil, 1 s.d.). Over the same time period, mean Hg concentrations in these samples increased from 131 ± 6 ng/L (1 s.d.) to 180 ± 28 ng/L (1 s.d.). Coupled with a previous study of Hg isotopic fractionation during AMDEs, these results suggest that Hg initially deposited to the local snowpack was subsequently reemitted during photochemical reduction reactions and ultimately accumulated on the frost flowers. As a result of this process, frost flowers may lead to enhanced local retention of Hg deposited during AMDEs and may increase Hg loading to the Arctic Ocean.

Bomb-tritium input function calculated from the details of the nuclear atmospheric bomb tests released by the UNSCEAR [2000]

Improving the representation of the hydrological cycle in Atmospheric General Circulation Models (AGCMs) is one of the main challenges in modeling the Earth's climate system. One way to evaluate model performance is to simulate the transport of water isotopes. Among those available, tritium (HTO) is an extremely valuable tracer, because its content in the different reservoirs involved in the water cycle (stratosphere, troposphere, ocean) varies by order of magnitude. Previous work incorporated natural tritium into LMDZ-iso, a version of the LMDZ general circulation model enhanced by water isotope diagnostics. Here for the first time, the anthropogenic tritium injected by each of the atmospheric nuclear-bomb tests between 1945 and 1980 has been first estimated and further implemented in the model; it creates an opportunity to evaluate certain aspects of LDMZ over several decades by following the bomb-tritium transient signal through the hydrological cycle. Simulations of tritium in water vapor and precipitation for the period 1950-2008, with both natural and anthropogenic components, are presented in this study. LMDZ-iso satisfactorily reproduces the general shape of the temporal evolution of tritium. However, LMDZ-iso simulates too high a bomb-tritium peak followed by too strong a decrease of tritium in precipitation. The too diffusive vertical advection in AGCMs crucially affects the residence time of tritium in the stratosphere. This insight into model performance demonstrates that the implementation of tritium in an AGCM provides a new and valuable test of the modeled atmospheric transport, complementing water stable isotope modeling.

Grain size distribution and bulk chemistry of eolian dust

Atmospheric dust samples collected along a transect off the West African coast have been investigated for their physical (grain-size distribution), mineralogical, and chemical (major elements) composition. On the basis of these data the samples were grouped into sets of samples that most likely originated from the same source area. In addition, shipboard-collected atmospheric meteorological data, modeled 4-day back trajectories for each sampling day and location, and Total Ozone Mapping Spectrometer aerosol index data for the time period of dust collection (February-March 1998) were combined and used to reconstruct the sources of the groups of dust samples. On the basis of these data we were able to determine the provenance of the various dust samples. It appears that the bulk of the wind-blown sediments that are deposited in the proximal equatorial Atlantic Ocean are transported in the lower level (>~900 hPa) NE trade wind layer, which is a very dominant feature north of the Intertropical Convergence Zone (ITCZ). However, south of the surface expression of the ITCZ, down to 5°S, where surface winds are southwesterly, we still collected sediments that originated from the north and east, carried there by the NE trade wind layer, as well as by easterly winds from higher altitudes. The fact that the size of the wind-blown dust depends not only on the wind strength of the transporting agent but also on the distance to the source hampers a direct comparison of the dust's size distributions and measured wind strengths. However, a comparison between eolian dust and terrigenous sediments collected in three submarine sediment traps off the west coast of NW Africa shows that knowledge of the composition of eolian dust is a prerequisite for the interpretation of paleorecords obtained from sediment cores in the equatorial Atlantic.

R-ArcticNet, A Regional Hydrographic Data Network for the Pan-Arctic Region (ISO-image of CD-ROM)

We describe the contemporary hydrography of the pan-Arctic land area draining into the Arctic Ocean, northern Bering Sea, and Hudson Bay on the basis of observational records of river discharge and computed runoff. The Regional Arctic Hydrographic Network data set, R-ArcticNET, is presented, which is based on 3754 recording stations drawn from Russian, Canadian, European, and U.S. archives. R-ArcticNET represents the single largest data compendium of observed discharge in the Arctic. Approximately 73% of the nonglaciated area of the pan-Arctic is monitored by at least one river discharge gage giving a mean gage density of 168 gages per 106 km2. Average annual runoff is 212 mm yr?1 with approximately 60% of the river discharge occurring from April to July. Gridded runoff surfaces are generated for the gaged portion of the pan-Arctic region to investigate global change signals. Siberia and Alaska showed increases in winter runoff during the 1980s relative to the 1960s and 1970s during annual and seasonal periods. These changes are consistent with observations of change in the climatology of the region. Western Canada experienced decreased spring and summer runoff.

Talos Dome Ice Core Deuterium Data

During the 1996 Programma Nazionale di Ricerche in Antartide-International Trans-Antarctic Scientific Expedition traverse, two firn cores were retrieved from the Talos Dome area (East Antarctica) at elevations of 2316 m (TD, 89 m long) and 2246 m (ST556, 19 m long). Cores were dated by using seasonal variations in non-sea-salt (nss) SO42- concentrations coupled with the recognition of tritium marker level (1965-1966) and nss SO42- spikes due to the most important volcanic events in the past (Pinatubo 1991, Agung 1963, Krakatoa 1883, Tambora 1815, Kuwae 1452, Unknown 1259). The number of annual layers recognized in the TD and ST556 cores was 779 and 97, respectively. The dD record obtained from the TD core has been compared with other East Antarctic isotope ice core records (Dome C EPICA, South Pole, Taylor Dome). These records suggest cooler climate conditions between the middle of 16th and the beginning of 19th centuries, which might be related to the Little Ice Age (LIA) cold period. Because of the high degree of geographical variability, the strongest LIA cooling was not temporally synchronous over East Antarctica, and the analyzed records do not provide a coherent picture for East Antarctica. The accumulation rate record presented for the TD core shows a decrease during part of the LIA followed by an increment of about 11% in accumulation during the 20th century. At the ST556 site, the accumulation rate observed during the 20th century was quite stable.