Browsing by Author "Lowe, DC"
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- Item14CH4 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, JPThe 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)
- ItemAtmospheric cycling of radiomethane and the "fossil fraction" of the methane source(European Geosciences Union, 2007-05-02) Lassey, KR; Lowe, DC; Smith, AMThe cycling of (CH4)-C-14 ("radiomethane") through the atmosphere has been strongly perturbed in the industrial era by the release of C-14-free methane from geologic reservoirs ("fossil methane" emissions), and in the nuclear era, especially since ca 1970, by the direct release of nucleogenic radiomethane from nuclear power facilities. Contemporary measurements of atmospheric radiomethane have been used to estimate the proportion of fossil methane in the global methane source ( the "fossil fraction"), but such estimates carry high uncertainty due to the ill-determined nuclear-power source. Guided by a mass-balance formulation in a companion paper, we apply a contemporary time series of atmospheric radiomethane to quantify both the fossil fraction and the strength of the nuclear power source. We deduce that 30.0 +/- 2.3% ( 1 s.d.) of the global methane source for 1986 2000 has fossil origin, a fraction which may include some C-14-depleted refractory carbon such as from aged peat deposits. Since this estimate depends upon the validity of assumptions underlying a linear regression model, it should be seen as providing a plausible re-estimate rather than a definitive revision. Such a fossil fraction would be much larger ( by 50%) than is commonly accepted, with implications for inventory compilation. The co-estimated strength of the global nuclear-power source of radiomethane is consistent with values inferred independently from local nuclear facilities. © 2007, European Geosciences Union
- ItemCentennial evolution of the atmospheric methane budget: what do the carbon isotopes tell us?(European Geosciences Union, 2007-05-02) Lassey, KR; Etheridge, DM; Lowe, DC; Smith, AM; Ferretti, DFLittle is known about how the methane source inventory and sinks have evolved over recent centuries. New and detailed records of methane mixing ratio and isotopic composition ((CH4)-C-12, (CH4)-C-13 and (CH4)-C-14) from analyses of air trapped in polar ice and firn can enhance this knowledge. We use existing bottom-up constructions of the source history, including "EDGAR"- based constructions, as inputs to a model of the evolving global budget for methane and for its carbon isotope composition through the 20th century. By matching such budgets to atmospheric data, we examine the constraints imposed by isotope information on those budget evolutions. Reconciling both (CH4)-C-12 and (CH4)-C-13 budgets with EDGAR-based source histories requires a combination of: a greater proportion of emissions from biomass burning and/or of fossil methane than EDGAR constructions suggest; a greater contribution from natural such emissions than is commonly supposed; and/or a significant role for active chlorine or other highly-fractionating tropospheric sink as has been independently proposed. Examining a companion budget evolution for (CH4)-C-14 exposes uncertainties in inferring the fossil-methane source from atmospheric (CH4)-C-14 data. Specifically, methane evolution during the nuclear era is sensitive to the cycling dynamics of "bomb C-14" ( originating from atmospheric weapons tests) through the biosphere. In addition, since ca. 1970, direct production and release of (CH4)-C-14 from nuclear-power facilities is influential but poorly quantified. Atmospheric (CH4)-C-14 determinations in the nuclear era have the potential to better characterize both biospheric carbon cycling, from photosynthesis to methane synthesis, and the nuclear-power source. © Author(s) 2007
- ItemIn search of in-situ radiocarbon in Law Dome ice and firn(Elsevier, 2000-10-01) Smith, AM; Levchenko, VA; Etheridge, DM; Lowe, DC; Hua, Q; Trudinger, CM; Zoppi, U; Elcheikh, AResults of AMS radiocarbon measurements on CO and CO2 separated from firn air directly pumped from the ice sheet, and on CO2 separated from air extracted from ice cores by a dry grating technique, are presented. The firn air samples and ice cores used in this study were collected from the region of Law Dome, Antarctica. No evidence of in-situ 14CO2 was found in the firn air samples or the ice core air samples from one site although a slight enhancement of 14CO above expected polar atmospheric concentrations was observed for some firn air samples. A clear in-situ 14CO2 signal for ice pre-dating the radiocarbon bomb pulse was found, however, in air samples extracted from an ice core from a second site. We compare these results and propose an hypothesis to explain this apparent contradiction. The degree to which in-situ 14C is released from the ice crystals during trapping and bubble formation is considered and discussed. The selectivity of the dry grating technique for the extraction of trapped atmospheric gases from ice cores is also discussed and compared with other methods. © 2000 Elsevier Science B.V
- ItemInstruments and methods: a novel method for obtaining very large ancient air samples from ablating glacial ice for analyses of methane radiocarbon(International Glaciological Society, 2008-03) Petrenko, VV; Severinghaus, JP; Brook, EJ; Muhle, J; Headly, M; Harth, CM; Schaefer, H; Reeh, N; Weiss, RF; Lowe, DC; Smith, AMWe present techniques for obtaining large (similar to 100 L STP) samples of ancient air for analysis of C-14 of methane ((CH4)-C-14) and other trace constituents. Paleoatmospheric (CH4)-C-14 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 ([CH4]) 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 N-15 of N-2, delta O-18 of O-2, delta O-18(ice) and [CH4] measurements. The [CH4] blank of the melt extractions was <4 ppb. Measurements of delta O-18 and delta N-15 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 [CH4]. Corrected [CH4] is elevated over expected values by up to 132 ppb for most samples, suggesting some in situ CH4 production in ice at this site. © 2008, International Glaciological Society
- ItemMeasurements 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, DMWe 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
- ItemMethane from the east Siberian Arctic Shelf(American Association for the Advancement of Science (AAAS), 2010-09-03) Petrenko, VV; Etheridge, DM; Weiss, RF; Brook, EJ; Schaefer, H; Severinghaus, JP; Smith, AM; Lowe, DC; Hua, Q; Riedel, K
- ItemA 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, EJWe 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