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[1] During our aerosol measurement program at Syowa Station, Antarctica, in 2004-2007, some low-visibility (haze) phenomena were observed during winter―spring under conditions with low winds and without drifting snow and fog. During "Antarctic haze" phenomena, the number concentration of aerosol particles and black carbon concentration increased by 1 to 2 orders higher relative to background conditions at Syowa Station, whereas surface O 3 concentration dropped simultaneously, especially after polar sunrise. Chemical analysis showed that major aerosol constituents in the haze phenomena were sea salt (e.g., Na + , Cl ― ). Trajectory analysis and the Navy Aerosol Analysis and Prediction System model showed that plumes from biomass burning in South America and southern Africa were transported to Syowa Station, on the Antarctic coast, because of the eastward (occasionally westward) approach of cyclones in the Southern Ocean and subsequent poleward flow. This poleward flow from midlatitudes of the plume and injection of sea-salt particles during the transport might engender Antarctic haze phenomena at Syowa Station. Differences of 0 3 concentration between the background and the haze conditions tended to be larger in spring (after polar sunrise) than in winter. Enhancement of sea-salt particles in the haze events can serve important roles in providing additional sources of reactive halogen species.

[1] Histories of atmospheric N2O concentration and its δ15N and δ18O were reconstructed for the period 1952–2001 on the basis of the analyses of firn air collected at the North Greenland Ice Core Project (NGRIP), Greenland, and Dome Fuji and H72, Antarctica. The N2O concentration increased from 290 ppbv in 1952 to 316 ppbv in 2001, which agrees well with the results from atmospheric observations and polar ice core analyses. The δ15N and δ18O showed a secular decrease, the respective values being 8.9 and 21.5‰ in 1952 and 7.0 and 20.5‰ in 2001. Their rates of change also varied, from about −0.02‰ yr−1 in the 1950s to about −0.04‰ yr−1 in 1960–2001 for δ15N, and from about 0‰ yr−1 to −0.02‰ yr−1 for δ18O. The isotopic budgetary calculations using a two-box model indicated that anthropogenic N2O emission from soils played a main role in the atmospheric N2O increase after industrialization, as well as that the average isotopic ratio of anthropogenic N2O has potentially been changed temporally.

This study assesses polar stratospheric nitrous oxide (N(2)O) and methane (CH(4)) data from the Improved Limb Atmospheric Spectrometer-II (ILAS-II) on board the Advanced Earth Observing Satellite-II (ADEOS-II) retrieved by the Version 1.4 retrieval algorithm. The data were measured between January and October 2003. Vertical profiles of ILAS-II volume mixing ratio (VMR) data are compared with data from two balloon-borne instruments, the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS-B) and the MkIV instrument, as well as with two satellite sensors, the Odin Sub-Millimetre Radiometer (SMR) for N(2)O and the Halogen Occultation Experiment (HALOE) for CH(4). Relative percentage differences between the ILAS-II and balloon/satellite data and their median values are calculated in 10-ppbv-wide bins for N(2)O (from 0 to 400 ppbv) and in 0.05-ppmv-wide bins for CH(4) (from 0 to 2 ppmv) in order to assess systematic differences between the ILAS-II and balloon/satellite data. According to this study, the characteristics of the ILAS-II Version 1.4 N(2)O and CH(4) data differ between hemispheres. For ILAS-II N(2)O VMR larger than 250 ppbv, the ILAS-II N(2)O agrees with the balloon/SMR N(2)O within +/- 20% in both hemispheres. The ILAS-II N(2)O in the VMR range from 30-50 to 250 ppbv (corresponding to altitudes of similar to 17-30 km in the Northern Hemisphere (NH, mainly outside the polar vortex) and similar to 13-21 km in the Southern Hemisphere (SH, mainly inside the polar vortex) is smaller by similar to 10-30% than the balloon/SMR N(2)O. For ILAS-II N(2)O VMR smaller than 30 ppbv (>similar to 21 km) in the SH, the differences between the ILAS-II and SMR N(2)O are within +/- 10 ppbv. For ILAS-II CH(4) VMR larger than 1 ppmv ( similar to 30 km) and the ILAS-II CH(4) for its VMR smaller than 1 ppmv (>similar to 25 km) only in the NH, are abnormally small compared to the balloon/satellite data.

[1] Temporal and latitudinal variations of vertical profiles of N2O isotopomers were observed in the stratosphere over Japan (39°N, 142°E), Sweden (68°N, 20°E), and Antarctica (69°N, 40°E) during the period between 1990 and 2001. Samples were collected with a balloon-borne cryogenic sampler and analyzed by mass spectrometry in the laboratory. Observed enrichment factors for heavier isotopomers (15N14N16O, 14N15N16O, and 14N14N18O) relative to 14N14N16O were nearly constant in the lower stratosphere (less than ∼22 km) but increased at higher altitudes (∼22–35 km) while showing seasonal and latitudinal differences. Enrichment factors during the photolysis and photo-oxidation of N2O were also obtained in laboratory experiments and compared with those observed. We found that in the higher-altitude region (1) fractionation of the isotopomers is mainly determined by photolysis, but is also affected by physical processes, (2) subsidence of air masses in the winter polar vortex induces the intrusion of an upper stratospheric air mass depleted in N2O, and (3) decay of the vortex in the local spring leads to rapid horizontal advection of midlatitude air masses. At lower altitudes, isotopomer ratios are determined by photolysis, photo-oxidation, and the mixing of air masses within the stratosphere or between the stratosphere and the troposphere. Secular trend of isotopomer profiles was not detectable over Japan during 11 years. Assuming that the lower stratospheric air over midlatitudes is exchanged with the troposphere, isotopomer ratios of the N2O “back-flux” from the stratosphere were estimated. These values can be used in the isotopomeric mass balance model to constrain the global N2O budget.

[1] Observations of aerosol constituents and acidic gases in the Antarctic area were carried out at Syowa (39.58°E, 69.00°S) in 1997 and 1998 and Dome Fuji stations (39.62°E, 77.37°S) in 1997. Sea-salt concentrations decreased to background levels in the summer at both Syowa (Na+, ≤4 nmol m−3) and Dome Fuji (Na+, ∼0.44 nmol m−3 on average). During the winter, blizzard and strong wind may cause an increase of sea-salt particles at Syowa, whereas long-range transport from the boundary layer at midlatitudes and coastal Antarctic regions may contribute significantly to the increase in sea-salt particles observed at Dome Fuji. Particulate Cl− and Br− are liberated preferentially from sea-salt particles at Syowa and Dome Fuji in the summer. The molar ratio of Cl−/Na+ and Br−/Na+ at Syowa decreased to ∼0.5 and ≈0, respectively, in summer. At Dome Fuji more Cl− tend to be liberated from sea-salt particles thorough heterogeneous NO3− formation. The concentrations of gaseous chlorine species (mostly HCl) and bromine species ranged from 0.2 to 5.3 nmol m−3 and below detection limit (BDL) to 1.5 nmol m−3, respectively, corresponding to sea-salt modification. In the present study, SO42− depletion due to mirabilite formation was observed not only at Syowa but also at Dome Fuji. This evidence suggests that SO42− depletion might occur through sublimation on snow surfaces in addition to seawater freezing. At Syowa, sea-salt fractionation relating to Mg2+, K+, and Ca2+ was also observed mostly under strong wind conditions.