Browsing by Author "Brailsford, G"

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    14CH4 measurements in Greenland ice: investigating last glacial termination CH4 sources
    (American Association for the Advancement of Science (AAAS), 2009-04-24) Petrenko, VV; Smith, AM; Brook, EJ; Lowe, DC; Riedel, K; Brailsford, G; Hua, Q; Schaefer, H; Reeh, N; Weiss, RF; Etheridge, DM; Severinghaus, JP
    The cause of a large increase of atmospheric methane concentration during the Younger Dryas-Preboreal abrupt climatic transition (~11,600 years ago) has been the subject of much debate. The carbon-14 (14C) content of methane (14CH4) should distinguish between wetland and clathrate contributions to this increase. We present measurements of 14CH4 in glacial ice, targeting this transition, performed by using ice samples obtained from an ablation site in west Greenland. Measured 14CH4 values were higher than predicted under any scenario. Sample 14CH4 appears to be elevated by direct cosmogenic 14C production in ice. 14C of CO was measured to better understand this process and correct the sample 14CH4. Corrected results suggest that wetland sources were likely responsible for the majority of the Younger Dryas-Preboreal CH4 rise. © 2009, American Association for the Advancement of Science (AAAS)
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    Early results from the ANSTO/NIWA 14C of atmospheric methane program
    (12th International Conference on Accelerator Mass Spectrometry (AMS-12), 2011-03-24) Smith, AM; Brailsford, G; Yang, B; Bromley, T; Martin, R
    development and proving of the laser heated microfurnace we have used it to prepare 45 samples of ~ 16 μg of carbon. These comprised CO2, derived from atmospheric methane, frozen back into glass breakseals following measurement for δ13C at NIWA. There were three sample sets: 15 from Baring Head, NZ (BHD), collected each ~ 15 days between March and September 2009, 9 from Arrival Heights, Antarctica (SCT), collected each ~ 41 days between February 2008 and January 2009, plus 21 samples taken along a Pacific Ocean voyage from Nelson (NZ) – Osaka (Japan) in December 2005 (FTW). All samples were measured to better than 1% precision, sufficient to reveal a 14CH4 signal. The BHD set shows significant temporal variation in 14C for baseline air passing over the Southern Ocean, whereas the SCT set shows a lesser variation for Antarctic air. The FTW set covers a S-N transect across the Pacific Ocean, showing the influence of the ITCZ (5°-10° N) and different meteorological conditions on the concentration, δ13C and Δ14C of CH4 and demonstrates that CH4 is not well mixed. Graphitisation reactions averaged 32 min with 0.7 mg of Fe, reduced from Fe2O3, as the catalyst. The samples, blanks and standards were measured in two 10 minute blocks; some were measured again to improve statistics. Average 13C4+ currents per microgram of carbon were 13, 4 and 2 nA/μg for each 10 min block. Similarly-sized targets prepared in the conventional furnace with Fe2O3 gave 8, 5 and 2 nA/μg for each 10 min block. Graphitisation efficiencies were typically 90-100% for microfurnace samples, compared with 37-84% for conventional furnace samples. Subsequent examination by microscope showed that the cesium beam was well-centred on the 1 mm diameter recess and that effectively all C/Fe was sputtered, leading to a (minimum) estimation of ~4% overall AMS measurement efficiency. Copyright (c) 2011 AMS12
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    Effect of N2O, catalyst, and means of water vapor removal on the graphitization of small CO2 samples.
    (University of Arizona, 2006-04-03) Smith, AM; Petrenko, VV; Hua, Q; Southon, J; Brailsford, G
    The effect of nitrous oxide (N2O) Upon the graphitization of small (similar to 40 mu g of carbon) CO2 samples at the ANSTO and University of California, Irvine, radiocarbon laboratories was investigated. Both laboratories produce graphite samples by reduction of CO2 over a heated iron catalyst in the presence of an excess of H-2. Although there are significant differences between the methods employed at each laboratory, it was found that N2O has no effect upon the reaction at levels of up to 9.3% by volume Of CO2. Further, it was systematically determined that more effective water vapor trapping resulted in faster reaction rates. Using larger amounts of the Fe catalyst generally resulted in higher yields or reaction rates (but not both). The effects of changing the type of Fe catalyst on the final yield and reaction rate were less clear.
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    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
    (Elsevier Science BV., 2013-03-01) Petrenko, VV; Severinghaus, JP; Smith, AM; Riedel, K; Baggenstos, D; Harth, CM; Orsi, AJ; Hua, Q; Franz, P; Takeshita, Y; Brailsford, G; Weiss, RF; Buizert, C; Dickson, A; Schaefer, H
    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. © 2013, Elsevier Ltd.
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    High-precision measurements of 14C in ice cores: results and future prospects
    (American Geophysical Union (AGU), 2012-12-03) Petrenko, VV; Severinghaus, JP; Smith, AM; Schaefer, H; Riedel, K; Brook, EJ; Buizert, C; Baggenstos, D; Harth, CM; Hua, Q; Orsi, AJ; Bauska, TK; Schilt, A; Mitchell, L; Faïn, X; Takeshita, Y; Lee, JE; Brailsford, G; Franz, P; Weiss, RF; Dickson, A
    Measurements of 14C 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 14C signals in ice is complicated by the fact that there is a poorly-understood in situ cosmogenic component in addition to the trapped atmospheric component. A new analytical system allowed 14C of CH4 in glacial ice to be measured for the first time and improved measurement precision for 14C of CO in ice by an order of magnitude over prior work. Measurements of 14C of CH4 in ablating Greenland ice suggested that wetlands were the likely main driver of the Younger Dryas - Preboreal rapid atmospheric CH4 rise ≈ 11,600 yr ago, but interpretation was complicated by what appeared to be an unexpected significant in situ cosmogenic 14CH4 component. Subsequent measurements in shallow firn at Greenland Summit and in 50-kyr-old ablating ice at Taylor Glacier, Antarctica ice definitively confirmed in situ cosmogenic 14CH4 production in glacial ice. The Taylor Glacier measurements also precisely quantified the in situ 14CH4 / 14CO ratio for muogenic 14C production (0.0078 ± 0.0001). The observed constancy of this ratio demonstrated that 14C of CO can be used to quantify the cosmogenic 14CH4 content, allowing for accurate reconstructions of the absolute paleo-atmospheric 14C of CH4 from glacial ice. Measurements in Greenland shallow firn clearly demonstrated that almost all in situ cosmogenic 14C is rapidly lost from the shallow firn to the atmosphere. This implies that 14C of CO2 at most ice core sites is dominated by the atmospheric component and, with a 14CO-based correction for the cosmogenic component, can likely be used for absolute dating of ice. Even given the rapid in-situ cosmogenic 14C loss in the firn, 14C of CO is still expected to be dominated by the cosmogenic component and is a promising tracer for past cosmic ray flux. © AGU 2012
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    Measurements of 14C in ancient ice from Taylor Glacier, Antarctica constrain in situ cosmogenic 14CH4 and 14CO production rates
    (Elsevier, 2016-03-15) Petrenko, VV; Severinghaus, JP; Schaefer, H; Smith, AM; Kuhl, TW; Baggenstos, D; Hua, Q; Brook, EJ; Rose, P; Kulin, R; Bauska, TK; Harth, CM; Buizert, C; Orsi, AJ; Emanuele, G; Lee, JE; Brailsford, G; Keeling, R; Weiss, RF
    Carbon-14 (14C) is incorporated into glacial ice by trapping of atmospheric gases as well as direct near-surface in situ cosmogenic production. 14C of trapped methane (14CH4) is a powerful tracer for past CH4 emissions from “old” carbon sources such as permafrost and marine CH4 clathrates. 14C in trapped carbon dioxide (14CO2) can be used for absolute dating of ice cores. In situ produced cosmogenic 14C in carbon monoxide (14CO) can potentially be used to reconstruct the past cosmic ray flux and past solar activity. Unfortunately, the trapped atmospheric and in situ cosmogenic components of 14C in glacial ice are difficult to disentangle and a thorough understanding of the in situ cosmogenic component is needed in order to extract useful information from ice core 14C. We analyzed very large (≈1000 kg) ice samples in the 2.26–19.53 m depth range from the ablation zone of Taylor Glacier, Antarctica, to study in situ cosmogenic production of 14CH4 and 14CO. All sampled ice is >50 ka in age, allowing for the assumption that most of the measured 14C originates from recent in situ cosmogenic production as ancient ice is brought to the surface via ablation. Our results place the first constraints on cosmogenic 14CH4 production rates and improve on prior estimates of 14CO production rates in ice. We find a constant 14CH4/14CO production ratio (0.0076 ± 0.0003) for samples deeper than 3 m, which allows the use of 14CO for correcting the 14CH4 signals for the in situ cosmogenic component. Our results also provide the first unambiguous confirmation of 14C production by fast muons in a natural setting (ice or rock) and suggest that the 14C production rates in ice commonly used in the literature may be too high. © 2016, Elsevier Ltd.
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    Measurements of carbon-14 of methane in Greenland ice: investigating methane sources during the Last Glacial Termination
    (American Geophysical Union (AGU), 2008-12-15) Petrenko, VV; Smith, AM; Severinghaus, JP; Brook, EJ; Lowe, DC; Riedel, K; Brailsford, G; Hua, Q; Reeh, N; Schaefer, H; Weiss, RF; Etheridge, DM
    We present the first measurements of 14C of methane (14CH4) in ancient glacial ice. 14CH4 should distinguish unambiguously between wetland and fossil (clathrate or other geologic CH4) contributions to abrupt atmospheric CH4 increases observed at times of rapid warming in Greenland ice cores. 1000-kg-sized ice samples, dating to the Younger Dryas - Preboreal (around 11,600 yr BP) and Oldest Dryas - Bølling (around 14,700 yr BP) abrupt climatic transitions, were obtained from an ablation site in West Greenland. Measured 14CH4 values (28 - 35 pMC) were higher than predicted under any scenario based on sample age. Sample 14CH4 appears to be elevated by in- situ CH4 production in the ice for some samples as well as by a second process that is likely direct cosmogenic production of 14CH4 molecules in the ice. 14C of CO and CO2 was measured to better understand these processes and corrections were applied to sample 14CH4. Although the corrected results have substantial uncertainties, they suggest that wetland sources were responsible for the majority of the Younger Dryas - Preboreal CH4 rise. The uncertainties in the corrected results for the Oldest Dryas - Bølling transition are too large to draw conclusions about 14CH4 changes during that transition. © 2008 American Geophysical Union
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    A new method for analyzing 14C of methane in ancient air extracted from glacial ice
    (University of Arizona, 2008-03) Petrenko, VV; Smith, AM; Brailsford, G; Riedel, K; Hua, Q; Lowe, DC; Severinghaus, JP; Levchenko, VA; Bromley, T; Moss, R; Muhle, J; Brook, EJ
    We present a new method developed for measuring radiocarbon of methane (14CH4) in ancient air samples extracted from glacial ice and dating 11,000–15,000 calendar years before present. The small size (~20 μg CH4 carbon), low CH4 concentrations ([CH4], 400–800 parts per billion [ppb]), high carbon monoxide concentrations ([CO]), and low 14C 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. 14C procedural blanks were greatly reduced through the construction of a new CH4 conversion line utilizing platinized quartz wool for CH4 combustion and the use of an ultra-high-purity iron catalyst for graphitization. The amount and 14C activity of extraneous carbon added in the new CH4 conversion line were determined to be 0.23 ± 0.16 μg 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 μg. The overall procedural blank for all stages of sample handling was 0.75 ± 0.38 pMC for ~20-μg, 14C-free air samples with [CH4] of 500 ppb. Duration of the graphitization reactions for small (<25 μg 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. 14C corrections for each step of sample handling have been determined. The resulting overall 14CH4 uncertainties for the ancient air samples are ~1.0 pMC. © 2008, University of Arizona