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Battle, MO, Severinghaus JP, Sofen ED, Plotkin D, Orsi AJ, Aydin M, Montzka SA, Sowers T, Tans PP.  2011.  Controls on the movement and composition of firn air at the West Antarctic Ice Sheet Divide. Atmospheric Chemistry and Physics. 11:11007-11021.   10.5194/acp-11-11007-2011   AbstractWebsite

We sampled interstitial air from the perennial snowpack (firn) at a site near the West Antarctic Ice Sheet Divide (WAIS-D) and analyzed the air samples for a wide variety of gas species and their isotopes. We find limited convective influence (1.4-5.2 m, depending on detection method) in the shallow firn, gravitational enrichment of heavy species throughout the diffusive column in general agreement with theoretical expectations, a similar to 10 m thick lock-in zone beginning at similar to 67 m, and a total firn thickness consistent with predictions of Kaspers et al. (2004). Our modeling work shows that the air has an age spread (spectral width) of 4.8 yr for CO2 at the firn-ice transition. We also find that advection of firn air due to the 22 cm yr(-1) ice-equivalent accumulation rate has a minor impact on firn air composition, causing changes that are comparable to other modeling uncertainties and intrinsic sample variability. Furthermore, estimates of 1 age (the gas age/ice age difference) at WAIS-D appear to be largely unaffected by bubble closure above the lock-in zone. Within the lock-in zone, small gas species and their isotopes show evidence of size-dependent fractionation due to permeation through the ice lattice with a size threshold of 0.36 nm, as at other sites. We also see an unequivocal and unprecedented signal of oxygen isotope fractionation within the lock-in zone, which we interpret as the mass-dependent expression of a size-dependent fractionation process.

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Buizert, C, Severinghaus JP.  2016.  Dispersion in deep polar firn driven by synoptic-scale surface pressure variability. Cryosphere. 10:2099-2111.   10.5194/tc-10-2099-20160   AbstractWebsite

Commonly, three mechanisms of firn air transport are distinguished: molecular diffusion, advection, and near-surface convective mixing. Here we identify and describe a fourth mechanism, namely dispersion driven by synoptic-scale surface pressure variability (or barometric pumping). We use published gas chromatography experiments on firn samples to derive the along-flow dispersivity of firn, and combine this dispersivity with a dynamical air pressure propagation model forced by surface air pressure time series to estimate the magnitude of dispersive mixing in the firn. We show that dispersion dominates mixing within the firn lock-in zone. Trace gas concentrations measured in firn air samples from various polar sites confirm that dispersive mixing occurs. Including dispersive mixing in a firn air transport model suggests that our theoretical estimates have the correct order of magnitude, yet may overestimate the true dispersion. We further show that strong barometric pumping, such as at the Law Dome site, may reduce the gravitational enrichment of delta N-15-N-2 and other tracers below gravitational equilibrium, questioning the traditional definition of the lock-in depth as the depth where delta N-15 enrichment ceases. Last, we propose that Kr-86 excess may act as a proxy for past synoptic activity (or paleo-storminess) at the site.

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Fain, X, Ferrari CP, Dommergue A, Albert MR, Battle M, Severinghaus J, Arnaud L, Barnola JM, Cairns W, Barbante C, Boutron C.  2009.  Polar firn air reveals large-scale impact of anthropogenic mercury emissions during the 1970s. Proceedings of the National Academy of Sciences of the United States of America. 106:16114-16119.   10.1073/pnas.0905117106   AbstractWebsite

Mercury (Hg) is an extremely toxic pollutant, and its biogeochemical cycle has been perturbed by anthropogenic emissions during recent centuries. In the atmosphere, gaseous elemental mercury (GEM; Hg degrees) is the predominant form of mercury (up to 95%). Here we report the evolution of atmospheric levels of GEM in mid- to high-northern latitudes inferred from the interstitial air of firn (perennial snowpack) at Summit, Greenland. GEM concentrations increased rapidly after World War II from approximate to 1.5 ng m(-3) reaching a maximum of approximate to 3 ng m(-3) around 1970 and decreased until stabilizing at approximate to 1.7 ng m(-3) around 1995. This reconstruction reproduces real-time measurements available from the Arctic since 1995 and exhibits the same general trend observed in Europe since 1990. Anthropogenic emissions caused a two-fold rise in boreal atmospheric GEM concentrations before the 1970s, which likely contributed to higher deposition of mercury in both industrialized and remotes areas. Once deposited, this toxin becomes available for methylation and, subsequently, the contamination of ecosystems. Implementation of air pollution regulations, however, enabled a large-scale decline in atmospheric mercury levels during the 1980s. The results shown here suggest that potential increases in emissions in the coming decades could have a similar large-scale impact on atmospheric Hg levels.