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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.

Huber, C, Beyerle U, Leuenberger M, Schwander J, Kipfer R, Spahni R, Severinghaus JP, Weiler K.  2006.  Evidence for molecular size dependent gas fractionation in firn air derived from noble gases, oxygen, and nitrogen measurements. Earth and Planetary Science Letters. 243:61-73.   10.1016/j.epsl.2005.12.036   AbstractWebsite

We present elemental and isotopic measurements of noble gases (He, Ne, Ar, Kr, and Xe), oxygen and nitrogen of firn air from two sites. The first set of samples was taken in 1998 at the summit of the Devon Ice Cap in the eastern part of Devon Island. The second set was taken in 2001 at NGRIP location (North Greenland). He and Ne are heavily enriched relative to Ar with respect to the atmosphere in the air near the close-off depth at around 50-70 in. The enrichment increases with depth and reaches the maximum value in the deepest samples just above the zone of impermeable ice where no free air could be extracted anymore. Similarly, elemental ratios of O(2)/N(2), O(2)/Ar and Ar/N(2) are increasing with depth. In contrast but in line with expectations, isotopic ratios of (15)N/(14)N, (18)O/(16)O, and (36)Ar/(40)Ar show no significant enrichment near the close-off depth. The observed isotopic ratios in the firn air column can be explained within the uncertainty ranges by the well-known processes of gravitational enrichment and thermal diffusion. To explain the elemental ratios, however, an additional fractionation process during bubble inclusion has to be considered. We implemented this additional process into our firn air model. The fractionation factors were found by fitting model profiles to the data. We found a very similar close-off fractionation behavior for the different molecules at both sites. For smaller gas species (mainly He and Ne) the fractionation factors are linearly correlated to the molecule size, whereas for diameters greater than about 3.6 A the fractionation seems to be significantly smaller or even negligible. An explanation for this size dependent fractionation process could be gas diffusion through the ice lattice. At Devon Island the enrichment at the bottom of the firn air column is about four times higher compared to NGRIP. We explain this by lower firn diffusivity at Devon Island, most probably due to melt layers, resulting in significantly reduced back diffusion of the excess gas near the close-off depth. The results of this study considerably increase the understanding of the processes occurring during air bubble inclusion near the close-off depth in firn and can help to improve the interpretation of direct firn air measurements, as well as air bubble measurements in ice cores, which are used in numerous studies as paleo proxies. (c) 2006 Elsevier B.V. All rights reserved.

Severinghaus, JP, Grachev A, Luz B, Caillon N.  2003.  A method for precise measurement of argon 40/36 and krypton/argon ratios in trapped air in polar ice with applications to past firn thickness and abrupt climate change in Greenland and at Siple Dome, Antarctica. Geochimica Et Cosmochimica Acta. 67:325-343.   10.1016/s0016-7037(02)00965-1   AbstractWebsite

We describe a method for measuring the (40)Ar/(36)Ar ratio and the (84)Kr/(36)Ar ratio in air from bubbles trapped in ice cores. These ratios can provide constraints on the past thickness of the firn layer at the ice core site and on the magnitude of past rapid temperature variations when combined with measured (15)N/(14)N. Both variables contribute to paleoclimatic studies and ultimately to the understanding of the controls on Earth's climate. The overall precision of the (40)Ar/(36)Ar method (1 standard error of the mean) is 0.012parts per thousand for a sample analyzed in duplicate, corresponding to +/-0.6 in in reconstructed firn thickness. We use conventional dynamic isotope ratio mass spectrometry with minor modifications and special gas handling techniques designed to avoid fractionation. About 100 g of ice is used for a duplicate pair of analyses. An example of the technique applied to the GISP2 ice core yields an estimate of 11 +/- 3K of abrupt warming at the end of the last glacial period 15,000 years ago. The krypton/argon ratio can provide a diagnostic of argon leakage out of the bubbles, which may happen (naturally) during bubble close-off or (artifactually) if samples are warmed near the freezing point during core retrieval or storage. Argon leakage may fractionate the remaining (40)Ar/(36)Ar ratio by +0.007parts per thousand per parts per thousand change in (84)Kr/(36)Ar, introducing a possible bias in reconstructed firn thickness of about +2 in if thermal diffusion is not accounted for or +6 in if thermal diffusion effects are quantified with measured (15)N/(14)N. Reproducibility of (84)Kr/(36)Ar measured in air is about +/-0.2parts per thousand (1 standard error of the mean) but is about +/-1parts per thousand for ice core samples. Ice core samples are systematically enriched in (84)Kr/(36)Ar relative to atmosphere by similar to5parts per thousand, probably reflecting preferential size-dependent exclusion of the smaller argon atom during bubble entrapment. Recent results from the Siple Dome ice core reveal two climate events during the last deglaciation, including an 18-in reduction in firn thickness associated with an abrupt warming at sometime between 18 and 22 kyr BP and a partial or total removal of the firn during an ablation event at 15.3 kyr BP. Copyright (C) 2003 Elsevier Science Ltd.

Severinghaus, JP, Grachev A, Battle M.  2001.  Thermal fractionation of air in polar firn by seasonal temperature gradients. Geochemistry Geophysics Geosystems. 2   10.1029/2000GC000146   AbstractWebsite

Air withdrawn from the top 5-15 m of the polar snowpack (fim) shows anomalous enrichment of heavy gases during summer, including inert gases. Following earlier work, we ascribe this to thermal diffusion, the tendency of a gas mixture to separate in a temperature gradient, with heavier molecules migrating toward colder regions. Summer warmth creates a temperature gradient in the top few meters of the firn due to the thermal inertia of the underlying firn and causes gas fractionation by thermal diffusion. Here we explore and quantify this process further in order to (1) correct for bias caused by thermal diffusion in firn air and ice core air isotope records, (2) help calibrate a new technique for measuring temperature change in ice core gas records based on thermal diffusion [Severinghaus et al., 1998], and (3) address whether air in polar snow convects during winter and, if so, whether it creates a rectification of seasonality that could bias the ice core record. We sampled air at 2-m-depth intervals from the top 15 m of the firn at two Antarctic sites, Siple Dome and South Pole, including a winter sampling at the pole. We analyzed (15)N/(14)N, (40)Ar/(36)Ar, (40)Ar/(38)Ar, (18)O/(16)O of O(2), O(2)/N(2), (84)Kr/(36)Ar, and (132)Xe/(36)Ar. The results show the expected pattern of fractionation and match a gas diffusion model based on first principles to within 30%. Although absolute values of thermal diffusion sensitivities cannot be determined from the data with precision, relative values of different gas pairs may. At Siple Dome, delta (40)Ar/4 is 66 +/- 2% as sensitive to thermal diffusion as delta (15)N, in agreement with laboratory calibration; delta (18)O/2 is 83 +/- 3%, and delta (84)Kr/48 is 33 +/- 3% as sensitive as delta (15)N. The corresponding figures for summer South Pole are 64 +/- 2%, 81 +/- 3%, and 34 +/- 3%. Accounting for atmospheric change, the figure for deltaO(2)/N(2)/4 is 90 +/- 3% at Siple Dome. Winter South Pole shows a strong depletion of heavy gases as expected. However, the data do not fit the model well in the deeper part of the profile and yield a systematic drift with depth in relative thermal diffusion sensitivities (except for Kr, constant at 34 +/- 4%), suggesting the action of some other process that is not currently understood. No evidence for wintertime convection or a rectifier effect is seen.

Severinghaus, JP, Keeling RF, Miller BR, Weiss RF, Deck B, Broecker WS.  1997.  Feasibility of using sand dunes as archives of old air. Journal of Geophysical Research-Atmospheres. 102:16783-16792.   10.1029/97jd00525   AbstractWebsite

Large unaltered samples of the atmosphere covering the past century would complement the history of atmospheric gases obtained from bubbles in ice cores, enabling measurement of geochemically important species such as O-2, (CH4)-C-14, and (CO)-C-14. Sand dunes are a porous media with interstitial air in diffusive contact with the atmosphere, somewhat analogous to the unconsolidated layer of firn atop glaciers. Recent studies have demonstrated the value of firn as an archive of old air [Battle et al., 1996; Bender et al., 1994a]. Unlike firn, sand dunes are incompressible and so remain permeable to greater depths and may extend the firn record into the past century. To evaluate the feasibility of using sand dunes as archives of old air, we drilled 60 m deep test holes in the Algodones Dunes, Imperial Valley, California. The main objective was to see if the air in a sand dune is as old as predicted by a diffusion model, or if the dune is rapidly flushed by advective pumping during windstorms and barometric pressure changes. We dated the air with chlorofluorocarbons and krypton-85, anthropogenic tracers whose atmospheric concentrations are known and have been increasing rapidly in the past half century. These tracer data match the pure diffusion model well, showing that advection in this dune is negligible compared to diffusion as a transport mechanism and that the mean age of the air at 61 m depth is similar to 10 years. Dunes therefore do contain old air. However, dunes appear to suffer from two serious drawbacks as archives. Microbial metabolism is evident in elevated CO2 and N2O and depressed CH4 and O-2 concentrations in this dune, corrupting the signals of interest in this and probably most dunes. Second, isotopic analyses of N-2 and O-2 from the dune show that fractionation of the gases occurs due to diffusion of water vapor, complicating the interpretation of the O-2 signal beyond the point of viability for an air archive. Sand dunes may be useful for relatively inert gases with large atmospheric concentration changes such as chlorofluorocarbons.