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Buizert, C, Baggenstos D, Jiang W, Purtschert R, Petrenko VV, Lu ZT, Muller P, Kuhl T, Lee J, Severinghaus JP, Brook EJ.  2014.  Radiometric Kr-81 dating identifies 120,000-year-old ice at Taylor Glacier, Antarctica. Proceedings of the National Academy of Sciences of the United States of America. 111:6876-6881.   10.1073/pnas.1320329111   AbstractWebsite

We present successful Kr-81-Kr radiometric dating of ancient polar ice. Krypton was extracted from the air bubbles in four similar to 350-kg polar ice samples from Taylor Glacier in the McMurdo Dry Valleys, Antarctica, and dated using Atom Trap Trace Analysis (ATTA). The Kr-81 radiometric ages agree with independent age estimates obtained from stratigraphic dating techniques with a mean absolute age offset of 6 +/- 2.5 ka. Our experimental methods and sampling strategy are validated by (i) Kr-85 and Ar-39 analyses that show the samples to be free of modern air contamination and (ii) air content measurements that show the ice did not experience gas loss. We estimate the error in the Kr-81 ages due to past geomagnetic variability to be below 3 ka. We show that ice from the previous interglacial period (Marine Isotope Stage 5e, 130-115 ka before present) can be found in abundance near the surface of Taylor Glacier. Our study paves the way for reliable radiometric dating of ancient ice in blue ice areas and margin sites where large samples are available, greatly enhancing their scientific value as archives of old ice and meteorites. At present, ATTA Kr-81 analysis requires a 40-80-kg ice sample; as sample requirements continue to decrease, Kr-81 dating of ice cores is a future possibility.

Petrenko, VV, Severinghaus JP, Smith AM, Riedel K, Baggenstos D, Harth C, Orsi A, Hua Q, Franz P, Takeshita Y, Brailsford GW, Weiss RF, Buizert C, Dickson A, Schaefer H.  2013.  High-precision C-14 measurements demonstrate production of in situ cosmogenic (CH4)-C-14 and rapid loss of in situ cosmogenic (CO)-C-14 in shallow Greenland firn. Earth and Planetary Science Letters. 365:190-197.   10.1016/j.epsl.2013.01.032   AbstractWebsite

Measurements of radiocarbon (C-14) in carbon dioxide (CO2), methane (CH4) and carbon monoxide (CO) from glacial ice are potentially useful for absolute dating of ice cores, studies of the past atmospheric CH4 budget and for reconstructing the past cosmic ray flux and solar activity. Interpretation of C-14 signals in ice is complicated by the fact that the two major C-14 components-trapped atmospheric and in situ cosmogenic-are present in a combined form, as well as by a very limited understanding of the in situ component. This study measured (CH4)-C-14 and (CO)-C-14 content in glacial firn with unprecedented precision to advance understanding of the in situ C-14 component. (CH4)-C-14 and (CO)-C-14 were melt-extracted on site at Summit, Greenland from three very large (similar to 1000 kg each) replicate samples of firn that spanned a depth range of 3.6-5.6 m. Non-cosmogenic C-14 contributions were carefully characterized through simulated extractions and a suite of supporting measurements. In situ cosmogenic (CO)-C-14 was quantified to better than +/- 0.6 molecules g(-1) ice, improving on the precision of the best prior ice (CO)-C-14 measurements by an order of magnitude. The (CO)-C-14 measurements indicate that most (>99%) of the in situ cosmogenic C-14 is rapidly lost from shallow Summit firn to the atmosphere. Despite this rapid C-14 loss, our measurements successfully quantified (CH4)-C-14 in the retained fraction of cosmogenic C-14 (to +/- 0.01 molecules g(-1) ice or better), and demonstrate for the first time that a significant amount of (CH4)-C-14 is produced by cosmic rays in natural ice. This conclusion increases the confidence in the results of an earlier study that used measurements of (CH4)-C-14 in glacial ice to show that wetlands were the likely main driver of the large and rapid atmospheric CH4 increase approximately 1 1.6 kyr ago. (C) 2013 Elsevier B.V. All rights reserved.

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.

Petrenko, VV, Smith AM, Brook EJ, Lowe D, Riedel K, Brailsford G, Hua Q, Schaefer H, Reeh N, Weiss RF, Etheridge D, Severinghaus JP.  2009.  14C-CH4 Measurements in Greenland Ice: Investigating Last Glacial Termination CH4 Sources. Science. 324:506-508.   10.1126/science.1168909   AbstractWebsite

The cause of a large increase of atmospheric methane concentration during the Younger Dryas-Preboreal abrupt climatic transition (similar to 11,600 years ago) has been the subject of much debate. The carbon-14 (C-14) content of methane ((CH4)-C-14) should distinguish between wetland and clathrate contributions to this increase. We present measurements of (CH4)-C-14 in glacial ice, targeting this transition, performed by using ice samples obtained from an ablation site in west Greenland. Measured (CH4)-C-14 values were higher than predicted under any scenario. Sample (CH4)-C-14 appears to be elevated by direct cosmogenic C-14 production in ice. C-14 of CO was measured to better understand this process and correct the sample (CH4)-C-14. Corrected results suggest that wetland sources were likely responsible for the majority of the Younger Dryas-Preboreal CH4 rise.

Grachev, AM, Brook EJ, Severinghaus JP, Pisias NG.  2009.  Relative timing and variability of atmospheric methane and GISP2 oxygen isotopes between 68 and 86 ka. Global Biogeochemical Cycles. 23   10.1029/2008gb003330   AbstractWebsite

The global biogeochemical cycle of methane has received wide attention because of methane's role as a greenhouse gas. Measurements of methane in air trapped in Greenland ice cores provide a high-resolution record of methane levels in the atmosphere over the past similar to 100 ka, providing clues about what controls the methane cycle on geologic timescales. Remarkable similarity between local temperature recorded in Greenland ice cores and changes in global methane concentrations has been noted in previous studies, with the inference that the local temperature variations have global significance, but the resolution of sampling and measurement precision limited fine-scale comparison of these variables. In this work a higher-precision (similar to 2 ppb) methane data set was obtained from the Greenland Ice Sheet Project 2 (GISP2) ice core for the time interval between 86 and 68 ka, encompassing three large abrupt warming events early in the last glacial period: Dansgaard-Oeschger (D-O) events 19, 20, and 21. The new data set consists of duplicate measurements at 158 depths, with average time resolution of 120 years. Such detailed measurements over D-O 21, the longest in Greenland records, have not yet been reported for other ice cores. The new data set documents short-term variability (similar to 20 ppb typical amplitude), which is remarkably persistent, and in many cases similar features are observed in the most detailed published delta(18)O(ice) record. High-precision GISP2 delta(15)N data show that changes in Greenland temperature are synchronous with the methane variations at the onset of D-O events 19, 20, and 21, supporting previous results from the Greenland Ice Core Project ice core for D-O 19 and 20. Cross-spectral analysis quantifies the extremely close similarity between the new methane record and the delta(18)O(ice) record. Because methane sources are widely distributed over the globe, this work further validates delta(18)O(ice) at Greenland summit as a geographically broad climate indicator on millennial to multicentennial timescales.

Petrenko, VV, Smith AM, Brailsford G, Riedel K, Hua Q, Lowe D, Severinghaus JP, Levchenko V, Bromley T, Moss R, Muhle J, Brook EJ.  2008.  A new method for analyzing (14)C of methane in ancient air extracted from glacial ice. Radiocarbon. 50:53-73. AbstractWebsite

We present a new method developed for measuring radiocarbon of methane ((14)CH(4)) in ancient air samples extracted from glacial ice and dating 11,000-15,000 calendar years before present. The small size (similar to 20 mu g CH(4) carbon), low CH(4) concentrations ([CH(4)], 400-800 parts per billion [ppb]), high carbon monoxide concentrations ([CO]), and low (14)C activity of the samples created unusually high risks of contamination by extraneous carbon. Up to 2500 ppb CO in the air samples was quantitatively removed using the Sofnocat reagent. (14)C procedural blanks were greatly reduced through the construction of a new CH(4) conversion line utilizing platinized quartz wool for CH(4) combustion and the use of an ultra-high-purity iron catalyst for graphitization. The amount and (14)C activity of extraneous carbon added in the new CH(4) conversion line were determined to be 0.23 +/- 0.16 pg and 23.57 +/- 16.22 pMC, respectively. The amount of modern (100 pMC) carbon added during the graphitization step has been reduced to 0.03 mu g. The overall procedural blank for all stages of sample handling was 0.75 0.38 pMC for similar to 20-mu g, (14)C-free air samples with [CH(4)] of 500 ppb. Duration of the graphitization reactions for small (<25 mu g C) samples was greatly reduced and reaction yields improved through more efficient water vapor trapping and the use of a new iron catalyst with higher surface area. (14)C corrections for each step of sample handling have been determined. The resulting overall (14)CH(4) uncertainties for the ancient air samples are similar to 1.0 pMC.

Grachev, AM, Brook EJ, Severinghaus JP.  2007.  Abrupt changes in atmospheric methane at the MIS 5b-5a transition. Geophysical Research Letters. 34   10.1029/2007gl029799   AbstractWebsite

New ice core analyses show that the prominent rise in atmospheric methane concentration at Dansgaard-Oeschger event 21 was interrupted by a century-long 20% decline, which was previously unrecognized. The reversal was found in a new similar to 100-year resolution study of methane in the GISP2 ice core, encompassing the beginning of D-O event 21, which also corresponds to the transition from MIS 5b to 5a. Although a corresponding reversal (within age uncertainty) is observed in climate proxies measured in GISP2 ice, including delta O-18(ice), electrical conductivity, light scattering, and several ions, this feature has not been discussed previously. Abrupt changes in methane are paralleled by changes in delta N-15 of trapped air, a quantity that reflects local temperature change at Greenland summit. The reversal described here supports the hypothesis that climate can be unstable during major transitions, as was previously described for the last deglaciation.

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.

Taylor, KC, White JWC, Severinghaus JP, Brook EJ, Mayewski PA, Alley RB, Steig EJ, Spencer MK, Meyerson E, Meese DA, Lamorey GW, Grachev A, Gow AJ, Barnett BA.  2004.  Abrupt climate change around 22 ka on the Siple Coast of Antarctica. Quaternary Science Reviews. 23:7-15.   10.1016/j.quascirev.2003.09.004   AbstractWebsite

A new ice core from Siple Dome, Antarctica suggests the surface temperature increased by similar to6degreesC in just several decades at approximately 22 ka BP. This abrupt change did not occur 500 kin away in the Byrd ice core, or in climate proxy records in the Siple Dome core indicative of the mid-latitude Pacific. This demonstrates there was significant spatial heterogeneity in the response of the Antarctic climate during the last deglaciation and draws attention to unexplained mechanisms of abrupt climate change in Antarctica. (C) 2003 Elsevier Ltd. All rights reserved.

Caillon, N, Severinghaus JP, Jouzel J, Barnola JM, Kang JC, Lipenkov VY.  2003.  Timing of atmospheric CO2 and Antarctic temperature changes across termination III. Science. 299:1728-1731.   10.1126/science.1078758   AbstractWebsite

The analysis of air bubbles from ice cores has yielded a precise record of atmospheric greenhouse gas concentrations, but the timing of changes in these gases with respect to temperature is not accurately known because of uncertainty in the gas age-ice age difference. We have measured the isotopic composition of argon in air bubbles in the Vostok core during Termination III (similar to240,000 years before the present). This record most likely reflects the temperature and accumulation change, although the mechanism remains unclear. The sequence of events during Termination III suggests that the CO2 increase tagged Antarctic deglacial warming by 800 +/- 200 years and preceded the Northern Hemisphere deglaciation.

Brook, EJ, Harder S, Severinghaus J, Steig EJ, Sucher CM.  2000.  On the origin and timing of rapid changes in atmospheric methane during the last glacial period. Global Biogeochemical Cycles. 14:559-572.   10.1029/1999gb001182   AbstractWebsite

We present high resolution records of atmospheric methane from the GISP2 (Greenland Ice Sheet Project 2) ice core for four rapid climate transitions that occurred during the past 50 ka: the end of the Younger Dryas at 11.8 ka, the beginning of the Bolling-Allerod period at 14.8 ka, the beginning of interstadial 8 at 38.2 ka, and the beginning of interstadial 12 at 45.5 ka. During these events, atmospheric methane concentrations increased by 200-300 ppb over time periods of 100-300 years, significantly more slowly than associated temperature and snow accumulation changes recorded in the ice core record. We suggest that the slower rise in methane concentration may reflect the timescale of terrestrial ecosystem response to rapid climate change. We find no evidence for rapid, massive methane emissions that might be associated with large-scale decomposition of methane hydrates in sediments. With additional results from the Taylor Dome Ice Core (Antarctica) we also reconstruct changes in the interpolar methane gradient tan indicator of the geographical distribution of methane sources) associated with some of the rapid changes in atmospheric methane. The results indicate that the rise in methane at the beginning of the Bolling-Allerod period and the later rise at the end of the Younger Dryas were driven by increases in both tropical and boreal methane sources. During the Younger Dryas (a 1.3 ka cold period during the last deglaciation) the relative contribution from boreal sources was reduced relative to the early and middle Holocene periods.