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2019
Baggenstos, D, Haberli M, Schmitt J, Shackleton SA, Birner B, Severinghaus JP, Kellerhals T, Fischer H.  2019.  Earth's radiative imbalance from the Last Glacial Maximum to the present. Proceedings of the National Academy of Sciences of the United States of America. 116:14881-14886.   10.1073/pnas.1905447116   AbstractWebsite

The energy imbalance at the top of the atmosphere determines the temporal evolution of the global climate, and vice versa changes in the climate system can alter the planetary energy fluxes. This interplay is fundamental to our understanding of Earth's heat budget and the climate system. However, even today, the direct measurement of global radiative fluxes is difficult, such that most assessments are based on changes in the total energy content of the climate system. We apply the same approach to estimate the long-term evolution of Earth's radiative imbalance in the past. New measurements of noble gas-derived mean ocean temperature from the European Project for Ice Coring in Antarctica Dome C ice core covering the last 40,000 y, combined with recent results from the West Antarctic Ice Sheet Divide ice core and the sea-level record, allow us to quantitatively reconstruct the history of the climate system energy budget. The temporal derivative of this quantity must be equal to the planetary radiative imbalance. During the deglaciation, a positive imbalance of typically +0.2 W.m(-2) is maintained for similar to 10,000 y, however, with two distinct peaks that reach up to 0.4 Wm(-2) during times of substantially reduced Atlantic Meridional Overturning Circulation. We conclude that these peaks are related to net changes in ocean heat uptake, likely due to rapid changes in North Atlantic deep-water formation and their impact on the global radiative balance, while changes in cloud coverage, albeit uncertain, may also factor into the picture.

Seltzer, AM, Ng J, Severinghaus JP.  2019.  Precise determination of Ar, Kr and Xe isotopic fractionation due to diffusion and dissolution in fresh water. Earth and Planetary Science Letters. 514:156-165.   10.1016/j.epsl.2019.03.008   AbstractWebsite

Dissolved noble gases are ideal conservative tracers of physical processes in the Earth system due to their chemical and biological inertness. Although bulk concentrations of dissolved Ar, Kr, and Xe are commonly measured to constrain physical models of atmosphere, ocean, and terrestrial hydrosphere processes, stable isotope ratios of these gases (e.g. Xe-136/Xe-129) are seldom used because of low signal-to-noise ratios. Here we present the first results from a new method of dissolved gas sampling, extraction and analysis that permits measurement of stable Ar, Kr, and Xe isotope ratios at or below similar to 5 per meg amu(-1) precision (1 sigma), two orders-of-magnitude below conventional Kr and Xe isotopic measurements. This gain in precision was achieved by quantitative extraction and subsequent purification of dissolved noble gases from 2-L water samples via helium sparging and viscous dual-inlet isotope ratio mass spectrometry. We have determined the solubility fractionation factors (alpha(sol)) for stable Ar, Kr, and Xe isotope ratios between similar to 2 and 20 degrees C via laboratory equilibration experiments. We have also conducted temperature-controlled air-water gas exchange experiments to estimate the kinetic fractionation factors (alpha(kin)) of these isotope ratios. We find that both alpha(sol) and alpha(kin), normalized by isotopic mass difference (Delta m), decrease in magnitude with atomic number but are proportional to Delta m for isotope ratios of the same element. With the new ability for high precision isotopic measurements, we suggest that dissolved Kr and Xe isotope ratios in groundwater represent a promising, novel geochemical tool with important applications for groundwater modeling, water resource management, and paleoclimate. (C) 2019 Elsevier B.V. All rights reserved.

2018
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, Shackleton S, Baggenstos D, Kawamura K, Severinghaus J.  2018.  Mean global ocean temperatures during the last glacial transition. Nature. 553:39-+.   10.1038/nature25152   AbstractWebsite

Little is known about the ocean temperature's long-term response to climate perturbations owing to limited observations and a lack of robust reconstructions. Although most of the anthropogenic heat added to the climate system has been taken up by the ocean up until now, its role in a century and beyond is uncertain. Here, using noble gases trapped in ice cores, we show that the mean global ocean temperature increased by 2.57 +/- 0.24 degrees Celsius over the last glacial transition (20,000 to 10,000 years ago). Our reconstruction provides unprecedented precision and temporal resolution for the integrated global ocean, in contrast to the depth-, region-, organism-and season-specific estimates provided by other methods. We find that the mean global ocean temperature is closely correlated with Antarctic temperature and has no lead or lag with atmospheric CO2, thereby confirming the important role of Southern Hemisphere climate in global climate trends. We also reveal an enigmatic 700-year warming during the early Younger Dryas period (about 12,000 years ago) that surpasses estimates of modern ocean heat uptake.

2008
Petrenko, VV, Severinghaus JP, Brook EJ, Muhle J, Headly M, Harth CM, Schaefer H, Reeh N, Weiss RF, Lowe D, Smith AM.  2008.  A novel method for obtaining very large ancient air samples from ablating glacial ice for analyses of methane radiocarbon. Journal of Glaciology. 54:233-244.   10.3189/002214308784886135   AbstractWebsite

We present techniques for obtaining large (similar to 100 L STP) samples of ancient air for analysis of (14)C of methane ((14)CH(4)) and other trace constituents. Paleoatmospheric (14)CH(4) measurements should constrain the fossil fraction of past methane budgets, as well as provide a definitive test of methane clathrate involvement in large and rapid methane concentration ([CH(4)]) increases that accompanied rapid warming events during the last deglaciation. Air dating to the Younger Dryas-Preboreal and Oldest Dryas-Bolling abrupt climatic transitions was obtained by melt extraction from old glacial ice outcropping at an ablation margin in West Greenland. The outcropping ice and occluded air were dated using a combination of delta(15)N of N(2), delta(18)O of O(2), delta(18)O(ice) and [CH(4)] measurements. The [CH(4)] blank of the melt extractions was <4 ppb. Measurements of delta(18)O and delta(15)N indicated no significant gas isotopic fractionation from handling. Measured Ar/N(2), CFC-11 and CFC-12 in the samples indicated no significant contamination from ambient air. Ar/N(2), Kr/Ar and Xe/Ar ratios in the samples were used to quantify effects of gas dissolution during the melt extractions and correct the sample [CH(4)]. Corrected [CH(4)] is elevated over expected values by up to 132 ppb for most samples, suggesting some in situ CH(4) production in ice at this site.

2003
Grachev, AM, Severinghaus JP.  2003.  Determining the thermal diffusion factor for Ar-40/Ar-36 in air to aid paleoreconstruction of abrupt climate change. Journal of Physical Chemistry A. 107:4636-4642.   10.1021/jp027817u   AbstractWebsite

The thermal diffusion factor (alpha(T)) of Ar-40/Ar-36 in air has been measured in the laboratory for the first time. The mean values of alpha(T) x 10(3) that we find at -30.0 degreesC are 9.85 +/- 0.04 for air and 11.25 +/- 0.03 for pure argon. The latter value is more precise than the data found in the literature. The temperature dependence of the thermal diffusion factor in air in the range -60 to -10 degreesC can be described by an empirical equation alpha(T) x 10(3) = 26.08 - 3952/ (+/-1%), where is the effective average temperature. Results of this study are valuable for reconstruction of magnitudes of abrupt climate change events recorded in Greenland ice cores. For one abrupt warming event similar to15,000 years ago, near the end of the last glacial period, these results yield a warming of 11 +/- 3 degreesC over several decades or less. Theoretical calculations are not yet able to provide the needed accuracy, and the experimental results for the thermal diffusion factor in air should be used for paleoenvironmental studies.

Grachev, AM, Severinghaus JP.  2003.  Laboratory determination of thermal diffusion constants for N-29(2)/N-28(2) in air at temperatures from-60 to 0 degrees C for reconstruction of magnitudes of abrupt climate changes using the ice core fossil-air paleothermometer. Geochimica Et Cosmochimica Acta. 67:345-360.   10.1016/s0016-7037(02)01115-8   AbstractWebsite

Rapid temperature change causes fractionation of isotopic gaseous species in air in firn (snow) by thermal diffusion, producing a signal that is preserved in trapped air bubbles as the snow forms ice. Using a model of heat penetration and gas diffusion in the firn, as well as the values of appropriate thermal diffusion constants, it is possible to reconstruct the magnitude of a particular paleoclimate change. Isotopic nitrogen in air serves as a convenient tracer for such paleoreconstruction, because the ratio N-29(2)/N-28(2) has stayed extremely constant in the atmosphere for greater than or equal to10(6) years. However, prior to this work no data were available for thermal diffusion of N-29(2)/N-28(2) in air, but only in pure N-2. We devised a laboratory experiment allowing fractionation of gases by thermal diffusion in a small, tightly controlled temperature difference. A mass spectrometer was employed in measuring the resulting fractionations yielding measurement precision greater than was attainable by earlier thermal diffusion investigators. Our laboratory experiments indicate that the value of the thermal diffusion sensitivity (Omega) for N-29(2)/N-28(2) in air is +(14.7 +/- 0.5) X 10(-3) per mil/degreesC when the average temperature is -30.0degreesC. The corresponding value for N-29(2)/N-28(2) in pure N-2 that we find is +(15.3 +/- 0.4) X 10(-3) per mil/degreesC at -30.6degreesC, in agreement with the previously available literature data within their large range of uncertainty. We find that an empirical equation, Omega = (8.656/T-K - 1232/T-K(2)) +/- 3% per mil/degreesC, describes the slight variation of the sensitivity values for N-29(2)/N-28(2) in air with temperature in the range of -60 to 0degreesC. A separate set of experiments also described in this paper rules out adsorption as a candidate for producing additional temperature change-driven fractionation of N-29(2)/N-28(2) in the firn air. The combined newly obtained data constitute a calibration of the fossil-air paleothermometer with respect to isotopic nitrogen and will serve to improve the estimates of the magnitudes of past abrupt climate changes recorded in ice cores. Copyright (C) 2003 Elsevier Science Ltd.

1996
Severinghaus, JP, Bender ML, Keeling RF, Broecker WS.  1996.  Fractionation of soil gases by diffusion of water vapor, gravitational settling, and thermal diffusion. Geochimica Et Cosmochimica Acta. 60:1005-1018.   10.1016/0016-7037(96)00011-7   AbstractWebsite

Air sampled from the moist unsaturated zone in a sand dune exhibits depletion in the heavy isotopes of N-2 and O-2. We propose that the depletion is caused by a diffusive flux of water vapor out of the dune, which sweeps out the other gases, forcing them to diffuse back into the dune. The heavy isotopes of N-2 and O-2 diffuse back more slowly, resulting in a steady-state depletion of the heavy isotopes in the dune interior. We predict the effect's magnitude with molecular diffusion theory and reproduce it in a laboratory simulation, finding good agreement between field, theory, and lab. The magnitude of the effect is governed by the ratio of the binary diffusivities against water vapor of a pair of gases, and increases similar to linearly with the difference between the water vapor mole fraction of the site and the advectively mixed reservoir with which it is in diffusive contact (in most cases the atmosphere). The steady-state effect is given by delta(i) = [i/j/i(0)/j(0) - 1] 10(3) parts per thousand congruent to [(1 - x(H2O)/1 - x(H2O0))((Dj-H2O/Di-H2O)-1) -1] 10(3) parts per thousand, where delta(i) is the fractional deviation in permil of the gas i/gas j ratio from the advectively mixed reservoir, x(H2O) and x(H2O0) are respectively the mole fractions of water vapor at the site and in the advectively mixed reservoir, and D-i-H2O is the binary diffusion coefficient of gas i with water vapor. The effect is independent of scale at steady state, but approaches steady state with the time constant of diffusion set by the length scale. Exploiting the mechanism, we make an experimental estimate of the relative diffusivities of O-2 and N-2 against water vapor, finding that O-2 diffuses 3.6 +/- 0.3% faster than N-2 despite its greater mass. We also confirm in the study dune the presence of two additional known processes: gravitational fractionation, heretofore seen only in the unconsolidated firn of polar ice sheets, and thermal diffusion, well described in laboratory studies but not seen previously in nature. We predict that soil gases in general will exhibit the three effects described here, the water vapor flux fractionation effect, gravitational fractionation, and thermal diffusion. However, our analysis neglects Knudsen diffusion and thus may be inapplicable to fine-grained soils.