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  • Cambridge University Press  (11)
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  • 1
    Publication Date: 2013-01-01
    Description: Establishing precise age-depth relationships of high-alpine ice cores is essential in order to deduce conclusive paleoclimatic information from these archives. Radiocarbon dating of carbonaceous aerosol particles incorporated in such glaciers is a promising tool to gain absolute ages, especially from the deepest parts where conventional methods are commonly inapplicable. In this study, we present a new validation for a published 14C dating method for ice cores. Previously 14C-dated horizons of organic material from the Juvfonne ice patch in central southern Norway (61.676°N, 8.354°E) were used as reference dates for adjacent ice layers, which were 14C dated based on their particulate organic carbon (POC) fraction. Multiple measurements were carried out on 3 sampling locations within the ice patch featuring modern to multimillennial ice. The ages obtained from the analyzed samples were in agreement with the given age estimates. In addition to previous validation work, this independent verification gives further confidence that the investigated method provides the actual age of the ice.
    Print ISSN: 0033-8222
    Electronic ISSN: 1945-5755
    Topics: Archaeology , Energy, Environment Protection, Nuclear Power Engineering , Geosciences
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  • 2
    Publication Date: 2019-07-22
    Description: Methane contributes substantially to global warming as the second most important anthropogenic greenhouse gas. Radiocarbon (14C) measurements of atmospheric methane can be used as a source apportionment tool, as they allow distinction between thermogenic and biogenic methane sources. However, these measurements remain scarce due to labor-intensive methods required. A new setup for the preparation of atmospheric methane samples for radiocarbon analysis is presented. The system combines a methane preconcentration line with a preparative gas chromatography technique to isolate pure methane samples for a compound-specific radiocarbon analysis. In order to minimize sample preparation time, we designed a simplified preconcentration line for the extraction of methane from 50 L atmospheric air, which corresponds to 50 µg C as required for a reliable 14C analysis of methane-derived CO2 gas measurement with accelerator mass spectrometry (AMS). The system guarantees a quantitative extraction of methane from atmospheric air samples for 14C analysis, with a good repeatability and a low processing blank. The setup was originally designed for the measurement of samples with low methane concentrations, but it can also be adapted to apportion sources from environmental compartments with high methane levels such as freshwaters or wetlands.
    Print ISSN: 0033-8222
    Electronic ISSN: 1945-5755
    Topics: Archaeology , Energy, Environment Protection, Nuclear Power Engineering , Geosciences
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  • 3
    Publication Date: 2019-05-20
    Description: Alpine glaciers are valuable archives for the reconstruction of human impact on the environment. Besides dating purposes, measurement of radiocarbon (14C) content provides a powerful tool for long-term source apportionment studies on the carbonaceous aerosols incorporated in ice cores. In this work, we present an extraction system for 14C analyses of dissolved organic carbon (DOC) in ice cores. The setup can process ice samples of up to 350 g mass and offers ultra-clean working conditions for all extraction steps. A photo-oxidation method is applied by means of external UV irradiation of the sample. For an irradiation time of 30 min with catalyzation by addition of Fe2+ and H2O2, we achieve an efficiency of 96 ± 6% on average. Inert gas working conditions and stringent decontamination procedures enable a low overall blank of 1.9 ± 1.6 μg C with a F14C value of 0.68 ± 0.13. This makes it possible to analyze the DOC in ice samples with a carbon content of as low as 25 μg C kg−1 ice. For a first validation, the new method was applied to ice core samples from the Swiss Alps. The average DOC concentration and F14C values for the Fiescherhorn ice core samples show good agreement with previously reported data for the investigated period of 1925–1936 AD.
    Print ISSN: 0033-8222
    Electronic ISSN: 1945-5755
    Topics: Archaeology , Energy, Environment Protection, Nuclear Power Engineering , Geosciences
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  • 4
    Publication Date: 2007-01-01
    Description: The novel tabletop miniaturized radiocarbon dating system (MICADAS) at ETH Zurich features a hybrid Cs sputter negative ion source for the measurement of solid graphite and gaseous CO2 samples. The source produces stable currents of up to 6 μA C− out of gaseous samples with an efficiency of 3–6%. A gas feeding system has been set up that enables constant dosing of CO2 into the Cs sputter ion source and ensures stable measuring conditions. The system is based on a syringe in which CO2 gas is mixed with He and then pressed continuously into the ion source at a constant flow rate. Minimized volumes allow feeding samples of 3–30 μg carbon quantitatively into the ion source. In order to test the performance of the system, several standards and blanks have successfully been measured. The ratios of 14C/12C could be repeated within statistical errors to better than 1.0% and the 13C/12C ratios to better than 0.2%. The blank was
    Print ISSN: 0033-8222
    Electronic ISSN: 1945-5755
    Topics: Archaeology , Energy, Environment Protection, Nuclear Power Engineering , Geosciences
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  • 5
    Publication Date: 2010-01-01
    Description: There is a great scientific demand for an assessment of the sources and formation processes of atmospheric carbonaceous aerosols since they strongly influence the global radiation balance and affect public health. Much attention in atmospheric studies has been paid to dicarboxylic acids (DCAs) due to their abundance at substantially different sites and their potential influence on cloud formation processes. Nevertheless, sources of oxalic acid (HOOCCOOH) and other DCAs are not well understood yet. In order to quantify contributions of fossil and non-fossil sources, a method for the preparative separation of oxalic acid and other DCAs from aerosols for compound-specific radiocarbon analysis (CSRA) has been developed. This method consists of a water extraction of aerosols collected on quartz-fiber filters followed by 2 consecutive liquid chromatography (LC) steps on different chromatography columns (2D-chromatography). Through the use of aqueous, completely non-organic eluents and single injections into liquid chromatography, low blank levels are achieved with total oxalic acid recoveries of up to 66%. Upon separation, 14C measurements of small samples (containing typically 10–20 μg carbon) are conducted at the gas ion source of the 200kV accelerator mass spectrometry facility MICADAS. The method is verified with processed reference materials, artificial mixtures of oxalic acid with typical matrix components, and a standard addition of ambient aerosols. Two exemplary field samples show dominant non-fossil sources of oxalic acid.
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    Electronic ISSN: 1945-5755
    Topics: Archaeology , Energy, Environment Protection, Nuclear Power Engineering , Geosciences
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  • 6
    Publication Date: 2013-01-01
    Description: Radiocarbon analysis of the carbonaceous aerosol allows an apportionment of fossil and non-fossil sources of airborne particulate matter (PM). A chemical separation of total carbon (TC) into its subtractions organic carbon (OC) and elemental carbon (EC) refines this powerful technique, as OC and EC originate from different sources and undergo different processes in the atmosphere. Although 14C analysis of TC, EC, and OC has recently gained increasing attention, interlaboratory quality assurance measures have largely been missing, especially for the isolation of EC and OC. In this work, we present results from an intercomparison of 9 laboratories for 14C analysis of carbonaceous aerosol samples on quartz fiber filters. Two ambient PM samples and 1 reference material (RM 8785) were provided with representative filter blanks. All laboratories performed 14C determinations of TC and a subset of isolated EC and OC for isotopic measurement. In general, 14C measurements of TC and OC agreed acceptably well between the laboratories, i.e. for TC within 0.015–0.025 F14C for the ambient filters and within 0.041 F14C for RM 8785. Due to inhomogeneous filter loading, RM 8785 demonstrated only limited applicability as a reference material for 14C analysis of carbonaceous aerosols. 14C analysis of EC revealed a large deviation between the laboratories of 28–79% as a consequence of different separation techniques. This result indicates a need for further discussion on optimal methods of EC isolation for 14C analysis and a second stage of this intercomparison.
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    Electronic ISSN: 1945-5755
    Topics: Archaeology , Energy, Environment Protection, Nuclear Power Engineering , Geosciences
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  • 7
    Publication Date: 2013-01-01
    Description: Radiocarbon offers a unique possibility for unambiguous source apportionment of carbonaceous particles due to a direct distinction of non-fossil and fossil carbon. In this work, particulate matter of different size fractions was collected at 4 sites in Switzerland to examine whether fine and coarse carbonaceous particles exhibit different fossil and contemporary sources. Elemental carbon (EC) and organic carbon (OC) as well as water-soluble OC (WSOC) and water-insoluble OC (WINSOC) were separated and determined for subsequent 14C measurement. In general, both fossil and non-fossil fractions in OC and EC were found more abundant in the fine than in the coarse mode. However, a substantial fraction (∼20 ± 5%) of fossil EC was found in coarse particles, which could be attributed to traffic-induced non-exhaust emissions. The contribution of biomass burning to coarse-mode EC in winter was relatively high, which is likely associated to the coating of EC with organic and/or inorganic substances emitted from intensive wood burning. Further, fossil OC (i.e. from vehicle emissions) was found to be smaller than non-fossil OC due to the presence of primary biogenic OC and/or growing in size of wood-burning OC particles during aging processes. 14C content in WSOC indicated that the second organic carbon rather stems from non-fossil precursors for all samples. Interestingly, both fossil and non-fossil WINSOC concentrations were found to be higher in fine particles than in coarse particles in winter, which is likely due to primary wood burning emissions and/or secondary formation of WINSOC.
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    Topics: Archaeology , Energy, Environment Protection, Nuclear Power Engineering , Geosciences
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  • 8
    Publication Date: 2004-01-01
    Description: Radiocarbon enables a distinction between contemporary and fossil carbon, which can be used for the apportionment of biogenic and anthropogenic sources in environmental studies. In order to apply this approach to carbonaceous atmospheric aerosols, it is necessary to adapt pretreatment procedures to the requirements of 14C measurements. In this work, we followed an approach in which total carbon (TC) is subdivided into fractions of different chemical and physical properties. 14C data of ambient aerosols from Zürich (Switzerland) are presented for the 2 sub-fractions of TC, organic carbon (OC) and elemental carbon (EC). Furthermore, OC is separated into water-insoluble OC (WINSOC) and water-soluble OC (WSOC). Results demonstrate the importance to differentiate between these fractions for 14C-deduced source apportionment, as the contributions can range between both extremes, nearly exclusively biogenic and anthropogenic.
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    Topics: Archaeology , Energy, Environment Protection, Nuclear Power Engineering , Geosciences
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  • 9
    Publication Date: 2010-01-01
    Description: An on-line measurement system was installed at the MICADAS in Zurich, using an elemental analyzer (EA) as a combustion unit to enable direct radiocarbon measurement of samples containing carbon in the range of 5–100 μg possible with minimum effort. The samples are combusted in small capsules and the gaseous combustion products are separated by the EA. The carbon dioxide leaving the EA in a high helium flow is concentrated on a small external trap containing X13 zeolite adsorber material. This new concept, avoiding a cryogenic trapping for the enrichment step, allows the construction of a very compact system able to work even with the smallest samples. Concentrated on the external trap, the carbon dioxide is flushed into the gas-tight syringe of our gas inlet system using a low helium stream. The gas mixture is measured with the MICADAS gas ion source. Several different sample capsules were analyzed to minimize the major blank contribution coming from the sample vessel. The best results were achieved with 25-μL tin capsules, which contained only 0.34 ± 0.13 μg carbon at 65 pMC. This work describes the development of the on-line system and the protocol for measurement runs. Results are presented for on-line measurements of reference materials and a comparison is performed with typical dating samples measured previously as graphite targets. Finally, relevance and limitations of on-line measurements are discussed.
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    Topics: Archaeology , Energy, Environment Protection, Nuclear Power Engineering , Geosciences
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  • 10
    Publication Date: 2020-05-26
    Description: We present the current performance of the in situ radiocarbon (14C) extraction line at the University of Bern with an improved extraction and combustion system. After three major steps of improvement, the extraction of sample CO2 gas now takes place inside a platinum crucible, supported by an outer quartz-glass crucible. This setup allows us to operate the line as a closed system for several samples without breaking the vacuum. Measurements of procedural blanks and samples from our reference strewn field, Jiddat al Harasis 073, performed in our system all show a good reproducibility and, for the strewn field samples, consistency with published data. We describe each improvement step in detail, discussing the advantages and disadvantages of all tested setups. By sharing our knowledge, we aim to inform and prevent others from making the same or similar detours in establishing 14C extraction systems for extraterrestrial samples.
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    Topics: Archaeology , Energy, Environment Protection, Nuclear Power Engineering , Geosciences
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