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Abstract: Reconstructions of past atmospheric concentrations of greenhouse gases provide unique insight into the biogeochemical cycles and the past radiative forcing in the Earth''s climate system. We present new measurements of atmospheric nitrous oxide along the ice cores of the North Greenland Ice Core Project and Talos Dome sites. Using records of several other ice cores, we are now able to establish the first complete composite nitrous oxide record reaching back to the beginning of the previous interglacial about 140,000yr ago. On the basis of such composite ice core records, we further calculate the radiative forcing of the three most important greenhouse gases carbon dioxide, methane and nitrous oxide during more than a full glacial–interglacial cycle. Nitrous oxide varies in line with climate, reaching very low concentrations of about 200 parts per billion by volume during Marine Isotope Stages 4 and 2, and showing substantial responses to millennial time scale climate variations during the last glacial. A large part of these millennial time scale variations can be explained by parallel changes in the sources of methane and nitrous oxide. However, as revealed by high-resolution measurements covering the Dansgaard/Oeschger events 17 to 15, the evolution of these two greenhouse gases may be decoupled on the centennial time scale. Carbon dioxide and methane concentrations do not reach interglacial levels in the course of millennial time scale climate variations during the last glacial. In contrast, nitrous oxide often reaches interglacial concentrations in response to both, glacial terminations and Dansgaard/Oeschger events. This indicates, from a biogeochemical point of view, similar drivers in both temporal cases. While carbon dioxide and methane concentrations are more strongly controlled by climate changes in high latitudes, nitrous oxide emissions changes may mainly stem from the ocean and/or from soils located at low latitudes. Accordingly, we speculate that high latitudes could play the leading role to trigger glacial terminations. [Copyright &y& Elsevier]

Abstract: We present records of atmospheric nitrous oxide obtained from the ice cores of the European Project for Ice Coring in Antarctica (EPICA) Dome C and Dronning Maud Land sites shedding light on the concentration of this greenhouse gas on glacial–interglacial and millennial time scales. The extended EPICA Dome C record covers now all interglacials of the last 800,000 years and reveals nitrous oxide variations in concert with climate. Highest mean interglacial nitrous oxide concentrations of 280 parts per billion by volume are observed during the interglacial corresponding to Marine Isotope Stage 11 around 400,000 years before present, at the same time when carbon dioxide and methane reach maximum mean interglacial concentrations. The temperature reconstruction at Dome C indicates colder interglacials between 800,000 and 440,000 years before present compared to the interglacials of the last 440,000 years. In contrast to carbon dioxide and methane, which both respond with lower concentrations at lower temperatures, nitrous oxide shows mean interglacial concentrations of 4–19 parts per billion by volume higher than the preindustrial Holocene value during the interglacials corresponding to Marine Isotope Stage 9–19. At the end of most interglacials, nitrous oxide remains substantially longer on interglacial levels than methane. Nevertheless, nitrous oxide shows millennial-scale variations at the same time as methane throughout the last 800,000 years. We suggest that these millennial-scale variations have been driven by a similar mechanism as the Dansgaard/Oeschger events known from the last glacial. Our data lead to the hypothesis that emissions from the low latitudes drive past variations of the atmospheric nitrous oxide concentration. [Copyright &y& Elsevier]

The atmospheric histories of two potent greenhouse gases, tetrafluoromethane (CF4) and hexafluoroethane (C2F6), have been reconstructed for the 20th century based on firn air measurements from both hemispheres. The reconstructed atmospheric trends show that the mixing ratios of both CF4 and C2F6 have increased during the 20th century by factors of ∼2 and ∼10, respectively. Initially, the increasing mixing ratios coincided with the rise in primary aluminum production. However, a slower atmospheric growth rate for CF4 appears to be evident during the 1990s, which supports recent aluminum industry reports of reduced CF4 emissions. This work illustrates the changing relationship between CF4 and C2F6 that is likely to be largely the result of both reduced emissions from the aluminum industry and faster growing emissions of C2F6 from the semiconductor industry. Measurements of C2F6 in the older firn air indicate a natural background mixing ratio of <0.3 parts per trillion (ppt), demonstrating that natural sources of this gas are negligible. However, CF4 was deduced to have a preindustrial mixing ratio of 34 ± 1 ppt (∼50% of contemporary levels). This is in good agreement with the previous work of Harnisch et al. (18) and provides independent confirmation of their results. As a result of the large global warming potentials of CF4 and C2F6, these results have important implications for radiative forcing calculations. The radiative forcings of CF4 and C2F6 are shown to have increased over the past 50 years to values in 2001 of 4.1 × 10-3 Wm-2 and 7.5 × 10-4 Wm-2, respectively, relative to preindustrial concentrations. These forcings are small compared to present day forcings due to the major greenhouse gases but, if the current trends continue, they will continue to increase since both gases have essentially infinite lifetimes. There is, therefore, a large incentive to reduce perfluorocarbon emissions such that, through the implementation of the Kyoto Protocol, the atmospheric growth rates may decline in the future. [ABSTRACT FROM AUTHOR]