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The seasonality of moisture sources for precipitation in Antarctica is studied with a Lagrangian moisture source diagnostic. Moisture origin for precipitation in Antarctica has strongly asymmetric properties, which are related to the Antarctic topography, seasonal sea ice coverage, and the land/ocean contrasts in the mid-latitudes of the southern hemisphere. The highest altitudes of the East Antarctic ice shield, where major ice cores have been drilled, have mean source latitudes of 45–40°S year-round. This finding contrasts to results from previous Lagrangian studies which detected a more southerly moisture origin due to too short trajectories. Now, results from Lagrangian moisture source diagnostics are consistent with findings from general circulation models with tagged tracers. Thus, both approaches can serve as a common benchmark for the interpretation of moisture source indicators based on stable isotopes, such as deuterium excess, in Antarctic ice cores.

We have developed a 5.5 year climatology of atmospheric transport into the Antarctic troposphere, which uses the same data set and methods as described in a recent study for the Arctic. This allows direct comparisons of transport properties for the two polar regions. The climatology is based on a simulation with the Lagrangian particle dispersion model FLEXPART, where the model atmosphere was globally filled with particles. Transport characteristics as well as emission sensitivities were derived from 6 hourly particle positions. We found that the probability for near-surface air to originate from the stratosphere on a time scale of 10 days is an order of magnitude higher near the South Pole than near the North Pole, a result of higher topography and descent that partly compensates for the flow of air down the Antarctic Plateau with the katabatic winds. The stratospheric influence is largest in fall, which is opposite to the seasonality in the Arctic. Stratospheric influence is much smaller over the shelf ice regions and in a band around Antarctica. The average time for which air near the surface has been exposed to continuous darkness in July (continuous light in January) is longest over the Ronne Ice Shelf and Ross Ice Shelf at ∼11 days (20 days). We calculated how sensitive Antarctic air masses are to emission input up to 30 days before arriving in Antarctica if removal processes are ignored. The emission sensitivity shows strong meridional gradients and, as a result, is generally low over South America, Africa, and Australia. For a 10 day time scale, the largest emission sensitivities over these continents are 1–2 orders of magnitude smaller than over Eurasia for transport to the Arctic, showing that foreign continents have a much smaller potential to pollute the Antarctic than the Arctic troposphere. Emission sensitivities and derived black carbon (BC) source contributions over South America, Africa, and Australia are substantially (a factor 10 for Africa) larger in winter than in summer. In winter, biomass burning contributes more BC than anthropogenic sources. For typical aerosol lifetimes of 5–10 days, ship emissions south of 60°S account for half of the total BC concentrations in the lowest 1000 m of the atmosphere south of 70°S in December. The increasing number of tourists visiting Antarctica and fishing vessels operating close to Antarctica are, therefore, a matter of concern.

The atmospheric observatory at the Norwegian Research Station Troll in Queen Maud Land, Antarctica, holds, since February 2007, the first all-year Antarctic atmospheric aerosol particle number size distribution measurements. These are colocated with measurements of the aerosol absorption and spectral scattering coefficients. In June 2007, this instrument set observed an aerosol whose properties were indicative of a biomass burning aerosol. These properties included two log-normal size distribution modes with median particle diameters of 0.105 μm and 0.36 μm, sharply falling off to smaller and larger sizes, and peaks in scattering and absorption coefficient. With backward plume calculations of the Lagrangian transport model FLEXPART and the MODIS fire activity product, a source-receptor relationship was established between biomass burning events in Central Brazil and the aerosol seen at Troll. This is the first direct evidence that the Antarctic continent is susceptible to emissions from as far north as Southern tropical latitudes.

Long term atmospheric mercury measurements in the Southern Hemisphere are scarce and in Antarctica completely absent. Recent studies have shown that the Antarctic continent plays an important role in the global mercury cycle. Therefore, long term measurements of gaseous elemental mercury (GEM) were initiated at the Norwegian Antarctic Research Station, Troll (TRS) in order to improve our understanding of atmospheric transport, transformation and removal processes of GEM. GEM measurements started in February 2007 and are still ongoing, and this paper presents results from the first four years. The mean annual GEM concentration of 0.93 ± 0.19 ng m−3 is in good agreement with other recent southern-hemispheric measurements. Measurements of GEM were combined with the output of the Lagrangian particle dispersion model FLEXPART, for a statistical analysis of GEM source and sink regions. It was found that the ocean is a source of GEM to TRS year round, especially in summer and fall. On time scales of up to 20 days, there is little direct transport of GEM to TRS from Southern Hemisphere continents, but sources there are important for determining the overall GEM load in the Southern Hemisphere and for the mean GEM concentration at TRS. Further, the sea ice and marginal ice zones are GEM sinks in spring as also seen in the Arctic, but the Antarctic oceanic sink seems weaker. Contrary to the Arctic, a strong summer time GEM sink was found, when air originates from the Antarctic plateau, which shows that the summertime removal mechanism of GEM is completely different and is caused by other chemical processes than the springtime atmospheric mercury depletion events. The results were corroborated by an analysis of ozone source and sink regions.

A first long-term monitoring of selected persistent organic pollutants (POPs) in Antarctic air has been conducted at the Norwegian research station Troll (Dronning Maud Land). As target contaminants 32 PCB congeners, α- and γ-hexachlorocyclohexane (HCH), trans- and cis-chlordane, trans- and cis-nonachlor, p,p'- and o,p-DDT, DDD, DDE as well as hexachlorobenzene (HCB) were selected. The monitoring program with weekly samples taken during the period 2007–2010 was coordinated with the parallel program at the Norwegian Arctic monitoring site (Zeppelin mountain, Ny-Ålesund, Svalbard) in terms of priority compounds, sampling schedule as well as analytical methods. The POP concentration levels found in Antarctica were considerably lower than Arctic atmospheric background concentrations. Similar to observations for Arctic samples, HCB is the predominant POP compound, with levels of around 22 pg m−3 throughout the entire monitoring period. In general, the following concentration distribution was found for the Troll samples analyzed: HCB > Sum HCH > Sum PCB > Sum DDT > Sum chlordanes. Atmospheric long-range transport was identified as a major contamination source for POPs in Antarctic environments. Several long-range transport events with elevated levels of pesticides and/or compounds with industrial sources were identified based on retroplume calculations with a Lagrangian particle dispersion model (FLEXPART).

An ongoing challenge in attributing anthropogenic climate change is to distinguish anthropogenic and natural changes of atmospheric composition, e.g. concerning atmospheric aerosol and its climate effects. Aerosol properties measured at pristine locations, to the extend they still exist, can serve as a climate model benchmark for verifying the representation of natural aerosol processes in the model.

This article investigates the annual cycle observed in the Antarctic baseline aerosol scattering coefficient, total particle number concentration, and particle number size distribution (PNSD), as measured at Troll Atmospheric Observatory. Mie theory shows that the annual cycles in microphysical and optical aerosol properties have a common cause. By comparison with observations at other Antarctic stations, it is shown that the annual cycle is not a local phenomenon, but common to central Antarctic baseline air masses. Observations of ground-level ozone at Troll as well as backward plume calculations for the air masses arriving at Troll demonstrate that the baseline air masses originate from the free troposphere and lower stratosphere region, and descend over the central Antarctic continent. The Antarctic summer PNSD is dominated by particles with diameters <100 nm recently formed from the gas-phase despite the absence of external sources of condensible gases. The total particle volume in Antarctic baseline aerosol is linearly correlated with the integral insolation the aerosol received on its transport pathway, and the photooxidative production of particle volume is mostly limited by photooxidative capacity, not availability of aerosol precursor gases. The photooxidative particle volume formation rate in central Antarctic baseline air is quantified to 207 ±4 μm3/(MJ m). Further research is proposed to investigate the applicability of this number to other atmospheric reservoirs, and to use the observed annual cycle in Antarctic baseline aerosol properties as a benchmark for the representation of natural atmospheric aerosol processes in climate models.

As part of the 2009 Operation Ice Bridge campaign, the NASA DC-8 aircraft was used to fill the data-time gap in laser observation of the changes in ice sheets, glaciers and sea ice between ICESat-I (Ice, Cloud, and land Elevation Satellite) and ICESat-II. Complementing the cryospheric instrument payload were four in situ atmospheric sampling instruments integrated onboard to measure trace gas concentrations of CO2, CO, N2O, CH4, water vapor and various VOCs (Volatile Organic Compounds). This paper examines two plumes encountered at high altitude (12 km) during the campaign; one during a southbound transit flight (13°S) and the other at 86°S over Antarctica. The data presented are especially significant as the Southern Hemisphere is heavily under-sampled during the austral spring, with few if any high-resolution airborne observations of atmospheric gases made over Antarctica. Strong enhancements of CO, CH4, N2O, CHCl3, OCS, C2H6, C2H2 and C3H8 were observed in the two intercepted air masses that exhibited variations in VOC composition suggesting different sources. The transport model FLEXPART showed that the 13°S plume contained predominately biomass burning emissions originating from Southeast Asia and South Africa, while both anthropogenic and biomass burning emissions were observed at 86°S with South America and South Africa as indicated source regions. The data presented here show evidence that boundary layer pollution is transported from lower latitudes toward the upper troposphere above the South Pole, which may not have been observed in the past.

New Zealand was among the last habitable places on earth to be colonized by humans. Charcoal records indicate that wildfires were rare prior to colonization and widespread following the 13th- to 14th-century Māori settlement, but the precise timing and magnitude of associated biomass-burning emissions are unknown, as are effects on light-absorbing black carbon aerosol concentrations over the pristine Southern Ocean and Antarctica. Here we used an array of well-dated Antarctic ice-core records to show that while black carbon deposition rates were stable over continental Antarctica during the past two millennia, they were approximately threefold higher over the northern Antarctic Peninsula during the past 700 years. Aerosol modelling demonstrates that the observed deposition could result only from increased emissions poleward of 40° S—implicating fires in Tasmania, New Zealand and Patagonia—but only New Zealand palaeofire records indicate coincident increases. Rapid deposition increases started in 1297 (±30 s.d.) in the northern Antarctic Peninsula, consistent with the late 13th-century Māori settlement and New Zealand black carbon emissions of 36 (±21 2 s.d.) Gg y−1 during peak deposition in the 16th century. While charcoal and pollen records suggest earlier, climate-modulated burning in Tasmania and southern Patagonia, deposition in Antarctica shows that black carbon emissions from burning in New Zealand dwarfed other preindustrial emissions in these regions during the past 2,000 years, providing clear evidence of large-scale environmental effects associated with early human activities across the remote Southern Hemisphere.