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Birner, B, Buizert C, Wagner TJW, Severinghaus JP.  2018.  The influence of layering and barometric pumping on firn air transport in a 2-D model. Cryosphere. 12:2021-2037.   10.5194/tc-12-2021-2018   AbstractWebsite

Ancient air trapped in ice core bubbles has been paramount to developing our understanding of past climate and atmospheric composition. Before air bubbles become isolated in ice, the atmospheric signal is altered in the firn column by transport processes such as advection and diffusion. However, the influence of low-permeability layers and barometric pumping (driven by surface pressure variability) on firn air transport is not well understood and is not readily captured in conventional one-dimensional (1-D) firn air models. Here we present a two-dimensional (2-D) trace gas advection-diffusion-dispersion model that accounts for discontinuous horizontal layers of reduced permeability. We find that layering or barometric pumping individually yields too small a reduction in gravitational settling to match observations. In contrast, when both effects are active, the model's gravitational fractionation is suppressed as observed. Layering focuses airflows in certain regions in the 2-D model, which acts to amplify the dispersive mixing resulting from barometric pumping. Hence, the representation of both factors is needed to obtain a realistic emergence of the lock-in zone. In contrast to expectations, we find that the addition of barometric pumping in the layered 2-D model does not substantially change the differential kinetic fractionation of fast-and slow-diffusing trace gases. Like 1-D models, the 2-D model substantially underestimates the amount of differential kinetic fractionation seen in actual observations, suggesting that further subgrid-scale processes may be missing in the current generation of firn air transport models. However, we find robust scaling relationships between kinetic isotope fractionation of different noble gas isotope and elemental ratios. These relationships may be used to correct for kinetic fractionation in future high-precision ice core studies and can amount to a bias of up to 0.45 degrees C in noble-gas-based mean ocean temperature reconstructions at WAIS Divide, Antarctica.

Bereiter, B, Kawamura K, Severinghaus JP.  2018.  New methods for measuring atmospheric heavy noble gas isotope and elemental ratios in ice core samples. Rapid Communications in Mass Spectrometry. 32:801-814.   10.1002/rcm.8099   AbstractWebsite

RationaleThe global ocean constitutes the largest heat buffer in the global climate system, but little is known about its past changes. The isotopic and elemental ratios of heavy noble gases (krypton and xenon), together with argon and nitrogen in trapped air from ice cores, can be used to reconstruct past mean ocean temperatures (MOTs). Here we introduce two successively developed methods to measure these parameters with a sufficient precision to provide new constraints on past changes in MOT. MethodsThe air from an 800-g ice sample - containing roughly 80mL STP air - is extracted and processed to be analyzed on two independent dual-inlet isotope ratio mass spectrometers. The primary isotope ratios (N-15, Ar-40 and Kr-86 values) are obtained with precisions in the range of 1 per meg (0.001) per mass unit. The three elemental ratio values Kr/N-2, Xe/N-2 and Xe/Kr are obtained using sequential (non-simultaneous) peak-jumping, reaching precisions in the range of 0.1-0.3. ResultsThe latest version of the method achieves a 30% to 50% better precision on the elemental ratios and a twofold better sample throughput than the previous one. The method development uncovered an unexpected source of artefactual gas fractionation in a closed system that is caused by adiabatic cooling and warming of gases (termed adiabatic fractionation) - a potential source of measurement artifacts in other methods. ConclusionsThe precisions of the three elemental ratios Kr/N-2, Xe/N-2 and Xe/Kr - which all contain the same MOT information - suggest smaller uncertainties for reconstructed MOTs (+/- 0.3-0.1 degrees C) than previous studies have attained. Due to different sensitivities of the noble gases to changes in MOT, Xe/N-2 provides the best constraints on the MOT under the given precisions followed by Xe/Kr, and Kr/N-2; however, using all of them helps to detect methodological artifacts and issues with ice quality.

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.

Rasmussen, SO, Abbott PM, Blunier T, Bourne AJ, Brook E, Buchardt SL, Buizert C, Chappellaz J, Clausen HB, Cook E, Dahl-Jensen D, Davies SM, Guillevic M, Kipfstuhl S, Laepple T, Seierstad IK, Severinghaus JP, Steffensen JP, Stowasser C, Svensson A, Vallelonga P, Vinther BM, Wilhelms F, Winstrup M.  2013.  A first chronology for the North Greenland Eemian Ice Drilling (NEEM) ice core. Climate of the Past. 9:2713-2730.   10.5194/cp-9-2713-2013   AbstractWebsite

A stratigraphy-based chronology for the North Greenland Eemian Ice Drilling (NEEM) ice core has been derived by transferring the annual layer counted Greenland Ice Core Chronology 2005 (GICC05) and its model extension (GICC05modelext) from the NGRIP core to the NEEM core using 787 match points of mainly volcanic origin identified in the electrical conductivity measurement (ECM) and dielectrical profiling (DEP) records. Tephra horizons found in both the NEEM and NGRIP ice cores are used to test the matching based on ECM and DEP and provide five additional horizons used for the timescale transfer. A thinning function reflecting the accumulated strain along the core has been determined using a Dansgaard-Johnsen flow model and an isotope-dependent accumulation rate parameterization. Flow parameters are determined from Monte Carlo analysis constrained by the observed depth-age horizons. In order to construct a chronology for the gas phase, the ice age-gas age difference (Delta age) has been reconstructed using a coupled firn densification-heat diffusion model. Temperature and accumulation inputs to the Delta age model, initially derived from the water isotope proxies, have been adjusted to optimize the fit to timing constraints from delta N-15 of nitrogen and high-resolution methane data during the abrupt onset of Greenland interstadials. The ice and gas chronologies and the corresponding thinning function represent the first chronology for the NEEM core, named GICC05modelext-NEEM-1. Based on both the flow and firn modelling results, the accumulation history for the NEEM site has been reconstructed. Together, the timescale and accumulation reconstruction provide the necessary basis for further analysis of the records from NEEM.

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.

Severinghaus, JP, Beaudette R, Headly MA, Taylor K, Brook EJ.  2009.  Oxygen-18 of O2 Records the Impact of Abrupt Climate Change on the Terrestrial Biosphere. Science. 324:1431-1434.   10.1126/science.1169473   AbstractWebsite

Photosynthesis and respiration occur widely on Earth's surface, and the O-18/O-16 ratio of the oxygen produced and consumed varies with climatic conditions. As a consequence, the history of climate is reflected in the deviation of the O-18/O-16 of air (delta O-18(atm)) from seawater delta O-18 (known as the Dole effect). We report variations in delta O-18(atm) over the past 60,000 years related to Heinrich and Dansgaard-Oeschger events, two modes of abrupt climate change observed during the last ice age. Correlations with cave records support the hypothesis that the Dole effect is primarily governed by the strength of the Asian and North African monsoons and confirm that widespread changes in low-latitude terrestrial rainfall accompanied abrupt climate change. The rapid delta O-18(atm) changes can also be used to synchronize ice records by providing global time markers.

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, Battle MO.  2006.  Fractionation of gases in polar lee during bubble close-off: New constraints from firn air Ne, Kr and Xe observations. Earth and Planetary Science Letters. 244:474-500.   10.1016/j.epsl.2006.01.032   AbstractWebsite

Gas ratios in air withdrawn from polar firn (snowpack) show systematic enrichments of Ne/N(2), O(2)/N(2) and Ar/N(2), in the firn-ice transition region where bubbles are closing off. Air from the bubbles in polar ice is correspondingly depleted in these ratios, after accounting for gravitational effects. Gas in the bubbles becomes fractionated during the process of bubble close-off and fractionation may continue as ice cores are stored prior to analysis. We present results from firn air studies at South Pole and Siple Dome, Antarctica, which add Ne, Kr and Xe measurements to the suite of observations. Ne, O(2) and Ar appear to be preferentially excluded from the shrinking and occluding bubbles, and these gases therefore accumulate in the residual firn air, creating a progressive enrichment with time (and depth) in firn air. Early sealing of gases by thin horizontal impermeable layers into a nondiffusive zone or "lock-in zone" greatly enhances this enrichment. A simple model of the bubble close-off fractionation and lock-in zone enrichment fits the data adequately. The model presumes that fractionation is caused by selective permeation of gas through the ice lattice from slightly overpressured bubbles. The effect appears to be size-dependent, because Ne, 02 and Ar have smaller effective molecular diameters than N(2), and fractionation increases strongly with decreasing size. Ne is fractionated 34 2 times more than 0, in South Pole firn air and reaches an enrichment of 90 parts per thousand in the deepest sample. The large atoms Kr and Xe do not appear to be fractionated by this process, despite the large size difference between the two gases, suggesting a threshold atomic diameter of similar to 3.6 angstrom above which the probability becomes very small that the gas will escape from the bubble. These findings have implications for ice core and firn air studies that use gas ratios to infer paleotemperature, chronology and past atmospheric composition. (c) 2006 Elsevier B.V.. All rights reserved.