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  • 1
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    Mass spectrometric method for the absolute calibration of the intramolecular nitrogen isotope distribution in nitrous oxide
    Springer Science and Business Media LLC ; 2004
    In:  Analytical and Bioanalytical Chemistry Vol. 378, No. 2 ( 2004-1-1), p. 256-269
    Details
    In: Analytical and Bioanalytical Chemistry, Springer Science and Business Media LLC, Vol. 378, No. 2 ( 2004-1-1), p. 256-269
    Type of Medium: Online Resource
    ISSN: 1618-2642 , 1618-2650
    URL: Article
    DOI: 10.1007/s00216-003-2233-2
    RVK:
    VA 4300
    Language: Unknown
    Publisher: Springer Science and Business Media LLC
    Publication Date: 2004
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  • 2
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    Isotopic enrichment of nitrous oxide ( 15 N 14 NO, 14 N 15 NO, 14 N 14 N 18 O) in the stratosphere and in the laboratory
    American Geophysical Union (AGU) ; 2001
    In:  Journal of Geophysical Research: Atmospheres Vol. 106, No. D10 ( 2001-05-27), p. 10403-10410
    Details
    In: Journal of Geophysical Research: Atmospheres, American Geophysical Union (AGU), Vol. 106, No. D10 ( 2001-05-27), p. 10403-10410
    Abstract: Nitrous oxide (N 2 O) extracted from stratospheric whole air samples has been analyzed for its 15 N and 18 O isotopic composition, and strong enrichments in the heavy isotopes are observed concomitant with decreasing N 2 O mixing ratio. Notably, the 15 N enrichment is strongly different at the two nonequivalent positions in the molecule. Laboratory broadband photolysis experiments at wavelengths representative for the stratosphere confirm that photolysis is the prime cause for the observed fractionation in the stratosphere. However, the in situ stratospheric fractionation constants are significantly reduced compared to the laboratory data, reflecting the importance of dynamic processes. In addition, small but significant variations in the ratio of the two 15 N fractionation constants indicate the influence of additional chemical processes like the oxidation of N 2 O by O( 1 D ).
    Type of Medium: Online Resource
    ISSN: 0148-0227
    URL: Article
    DOI: 10.1029/2000JD900822
    Language: English
    Publisher: American Geophysical Union (AGU)
    Publication Date: 2001
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  • 3
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    Why not take the train? Trans‐Siberian atmospheric chemistry observations across central and East Asia
    American Geophysical Union (AGU) ; 2002
    In:  Eos, Transactions American Geophysical Union Vol. 83, No. 45 ( 2002-11-05), p. 509-516
    Details
    In: Eos, Transactions American Geophysical Union, American Geophysical Union (AGU), Vol. 83, No. 45 ( 2002-11-05), p. 509-516
    Abstract: With an area of ∼17 million square km (almost 10% of the world's land area), Russia is of considerable importance for the global atmosphere and its changes. Its ecosystems encompass 25% of the world's forest area (about 10% of the global biomass [ Nilsson and Shvidenko , 1997]) and more than 25% of the global wetlands area [ Aselmann and Crutzen , 1989]. Furthermore, Russia covers an area that is sensitive to climate changes. We highlight the following most significant features of Russian ecosystems: The wetlands are of special importance, not only as natural sources of atmospheric methane (60–175 Tg yr 1 [ Aselmann and Crutzen , 1989]), but also because large oil and natural gas fields are being exploited there. Repeatedly there have been speculations about large losses of natural gas being of significance for the global atmospheric methane budget (∼35–95 Tg yr 1 [ Lelieveld et al. , 1998]).
    Type of Medium: Online Resource
    ISSN: 0096-3941 , 2324-9250
    URL: Article
    DOI: 10.1029/2002EO000351
    Language: English
    Publisher: American Geophysical Union (AGU)
    Publication Date: 2002
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  • 4
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    Gas chromatography/isotope-ratio mass spectrometry method for high-precision position-dependent 15 N and 18 O measurements of atmospheric nitrous oxide : High-precision position-dependent 15 N and 18 O measurements of N 2 O
    Wiley ; 2003
    In:  Rapid Communications in Mass Spectrometry Vol. 17, No. 16 ( 2003-08-30), p. 1897-1908
    Details
    In: Rapid Communications in Mass Spectrometry, Wiley, Vol. 17, No. 16 ( 2003-08-30), p. 1897-1908
    Type of Medium: Online Resource
    ISSN: 0951-4198
    URL: Article
    DOI: 10.1002/rcm.1132
    Language: English
    Publisher: Wiley
    Publication Date: 2003
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  • 5
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    Inverse modeling of the global CO cycle: 2. Inversion of 13 C/ 12 C and 18 O/ 16 O isotope ratios
    American Geophysical Union (AGU) ; 2000
    In:  Journal of Geophysical Research: Atmospheres Vol. 105, No. D2 ( 2000-01-27), p. 1929-1945
    Details
    In: Journal of Geophysical Research: Atmospheres, American Geophysical Union (AGU), Vol. 105, No. D2 ( 2000-01-27), p. 1929-1945
    Abstract: Following a three‐dimensional inverse modeling study on atmospheric CO mixing ratios [ Bergamaschi et al ., this issue], we present the expansion of our model for the treatment of the stable isotope ratios 13 C/ 12 C and 18 O/ 16 O in carbon monoxide. The individual isotopomers were included in the model as independent tracers, and the inversion scheme was extended, allowing the simultaneous optimization (with respect to observational data) of modeled atmospheric mixing and isotope ratios. Observational data of 13 C/ 12 C and 18 O/ 16 O ratios were taken from a set of five globally distributed sites, all of which exhibit pronounced seasonal cycles and which as a whole clearly define large latitudinal gradients. Incorporation of 13 C/ 12 C ratios in the inversion resulted in a clear constraining of the total amount of CO arising from CH 4 oxidation. The present study suggests an average CO yield of 86% (80–88%), provided that (1) the reaction of CH 4 +Cl has no significant impact on the δ 13 C of the resulting CO and (2) CO from the ocean helps to balance the δ 13 C in the Southern Hemisphere. Otherwise, a further reduced CO yield would be necessary, as low as 71% in case of an average kinetic isotope effect of 1.013 [ Lowe et al ., 1999] or 69% in case of a δ 13 C value of −25.0‰ for the oceanic source. Despite a lack of experimental investigations on 18 O/ 16 O in CO arising from CH 4 or nonmethanehydrocarbons (NMHC) oxidation, inclusion of 18 O/ 16 O into the inversion gives further significant constraints on the global CO cycle. It is shown that apart from the large technological CO source, additional sources with dominant emissions in the Northern Hemisphere are required, such as biogenic emissions (either direct or via oxidation of biogenic NMHCs) or anthropogenic NMHCs, in order to reproduce observed atmospheric 18 O/ 16 O ratios. The extended inversion scheme allows CO budgets to be derived, which reproduce, within two standard deviations of observational data, simultaneously CO mixing ratios (from the National Oceanic and Atmospheric Administration Climate Monitoring and Diagnostics Laboratory network), 13 C/ 12 C, and 18 O/ 16 O ratios. Incorporation of stable isotopes renders inversion results much more robust compared to inversions of CO mixing ratios only.
    Type of Medium: Online Resource
    ISSN: 0148-0227
    URL: Article
    DOI: 10.1029/1999JD900819
    Language: English
    Publisher: American Geophysical Union (AGU)
    Publication Date: 2000
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  • 6
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    On the 17 O correction for CO 2 mass spectrometric isotopic analysis
    Wiley ; 2003
    In:  Rapid Communications in Mass Spectrometry Vol. 17, No. 10 ( 2003-05-30), p. 1007-1016
    Details
    In: Rapid Communications in Mass Spectrometry, Wiley, Vol. 17, No. 10 ( 2003-05-30), p. 1007-1016
    Abstract: To calculate δ 13 C from raw CO 2 isotope data, the ion beam ratio of m/z 45 to 44 is corrected for the contribution arising from the contribution of 17 O‐bearing molecules. First, a review on the current state of 17 O‐corrections for CO 2 mass spectrometry is presented. The three correction algorithms that are generally in use, however, do produce biased δ 13 C values, and the bias is actually larger than the precision of modern isotope ratio mass spectrometers. The origin of this bias is twofold: different values for 17 R VPDB‐CO2 as well as different values for λ are used in the correction algorithms. Despite both values being of high importance, large discrepancies between the absolute values published for 17 R VPDB‐CO2 appear to be the main reason for the δ 13 C biases. Next, the question of how to choose the value of λ to best be used is considered. Natural (e.g. tropospheric) CO 2 as well as primary reference materials (PDB and NBS‐19), having been in isotope exchange with water, are assumed to lie on the fractionation line for waters. On this ground, λ  = 0.5281 ± 0.0015, as determined for waters (Meijer and Li, Isot. Environ. Health Stud. , 1998; 34: 349–369), is suggested to be a base for the 17 O‐correction algorithm. Finally, an approach to determine the absolute value for 17 R VPDB‐CO2 , based on data of relative isotope measurements on two CO 2 gases having a large 17 O difference, is discussed and algebraic formulas are considered. Experimental data and new numerical values determined for 17 R VPDB‐CO2 and 17 R VSMOW are given in a companion paper. Copyright © 2003 John Wiley & Sons, Ltd.
    Type of Medium: Online Resource
    ISSN: 0951-4198 , 1097-0231
    URL: Issue
    URL: Article
    DOI: 10.1002/rcm.v17:10
    DOI: 10.1002/rcm.1012
    Language: English
    Publisher: Wiley
    Publication Date: 2003
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  • 7
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    A redetermination of absolute values for 17 R VPDB‐CO2 and 17 R VSMOW
    Wiley ; 2003
    In:  Rapid Communications in Mass Spectrometry Vol. 17, No. 10 ( 2003-05-30), p. 1017-1029
    Details
    In: Rapid Communications in Mass Spectrometry, Wiley, Vol. 17, No. 10 ( 2003-05-30), p. 1017-1029
    Abstract: In a companion paper in this issue we presented a review of the current state of 17 O‐corrections for CO 2 mass spectrometry and considered an approach (including algebraic formulae) of how to determine absolute values for 17 R VPDB‐CO2 and 17 R VSMOW . Here we present the results of experiments conducted to determine these values. Two oxygen gases (one depleted in heavy isotopes and the other isotopically normal oxygen) were analysed to obtain the relative 17 O content. Samples of both gases were converted into CO 2 , and the resulting CO 2 samples were analysed as well. Possible experimental and analytical errors are carefully considered and eliminated as far as feasible. Much attention was paid to understanding and dealing with cross‐contamination effects occurring in the mass spectrometer. Based on the data obtained, the absolute values are calculated to be: 17 R VPDB‐CO2  = 0.00039511 ± 0.00000094 and 17 R VSMOW  = 0.00038672 ± 0.00000087 (expanded uncertainties). Both values are on the original scale of Craig ( Geochim. Cosmochim. Acta 1957; 12: 133–149) with 13 R VPDB‐CO2  = 0.0112372. A 17 O‐correction algorithm incorporating the newly determined value for 17 R VPDB‐CO2 and λ  = 0.528 by Meijer and Li ( Isot. Environ. Health Stud. 1998; 34: 349–369) is constructed. A computational test is performed to demonstrate the degree of δ 13 C bias relative to the previously known correction algorithms. δ 13 C values produced by the constructed algorithm are in the middle of the values produced by the other algorithms. We refrain, however, from giving any recommendation concerning which 17 O‐correction algorithm to use in order to obtain δ 13 C data in the most accurate way. The present work illuminates the need to reconsider recommendations concerning the correction algorithm. Copyright © 2003 John Wiley & Sons, Ltd.
    Type of Medium: Online Resource
    ISSN: 0951-4198 , 1097-0231
    URL: Issue
    URL: Article
    DOI: 10.1002/rcm.v17:10
    DOI: 10.1002/rcm.1011
    Language: English
    Publisher: Wiley
    Publication Date: 2003
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  • 8
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    Aerosol elemental concentrations in the tropopause region from intercontinental flights with the Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container (CARIBIC) platform : CARIBIC
    American Geophysical Union (AGU) ; 2002
    In:  Journal of Geophysical Research: Atmospheres Vol. 107, No. D23 ( 2002-12-16), p. AAC 3-1-AAC 3-14
    Details
    In: Journal of Geophysical Research: Atmospheres, American Geophysical Union (AGU), Vol. 107, No. D23 ( 2002-12-16), p. AAC 3-1-AAC 3-14
    Type of Medium: Online Resource
    ISSN: 0148-0227
    URL: Article
    DOI: 10.1029/2002JD002344
    Language: English
    Publisher: American Geophysical Union (AGU)
    Publication Date: 2002
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  • 9
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    Measurements of the carbon and hydrogen isotopes of atmospheric methane at Izaña, Tenerife: Seasonal cycles and synoptic‐scale variations
    American Geophysical Union (AGU) ; 2000
    In:  Journal of Geophysical Research: Atmospheres Vol. 105, No. D11 ( 2000-06-16), p. 14531-14546
    Details
    In: Journal of Geophysical Research: Atmospheres, American Geophysical Union (AGU), Vol. 105, No. D11 ( 2000-06-16), p. 14531-14546
    Abstract: Atmospheric CH 4 and its stable isotope ratios 13 C/ 12 C and D/H have been investigated at the Global Atmospheric Watch station Izaña, Tenerife (28°N, 16°W, 2370 m above sea level), since late 1996. Every fortnight both spot samples and integral samples were taken, the latter collected continuously over 2‐week periods. While spot samples show considerable synoptic‐scale variability, the continuous samples clearly define seasonal cycles of CH 4 , δ 13 C, and δD, with peak‐to‐peak amplitudes of 30 ppb, 0.2‰ and 3.5‰, respectively. The measurement of the δD seasonality is the first ever reported for atmospheric background CH 4 and has been made possible by the development of a tunable diode laser based optical Methane Isotopomer Spectrometer (MISOS). The δD is well in phase with CH 4 mixing ratios, and the compact correlation between them allows to derive the average kinetic isotope effect (KIE) of the tropospheric sinks to be 1.23±0.04 (1σ), consistent with recent laboratory measurements of the kinetic isotope effect in the reaction of CH 4 ±OH. In contrast to δD, δ 13 C is out of phase to CH 4 mixing ratios, clearly indicating that δ 13 C is not only effected by the KIE of the CH 4 ±OH reaction, but also by seasonally varying source mixtures. Considerable short‐term variations are observed in the isotopic composition and mixing ratios of the spot samples. This can be attributed to different origin of air masses arriving at Izaña. Significant CH 4 enhancement is observed for air masses originating from the North American continent or Europe, of 12.7±11.7 and 13.4±0.3 ppb, respectively, while air from the African continent or the North Atlantic is depleted (−11.2±2.8 and −7.0 ± 8.2 ppb). Deviations from the mean seasonal CH 4 cycle are correlated with significant deviations of δ 13 C and δD, allowing to estimate the δ 13 C and δD signatures of major source regions. Furthermore, deviations in CH 4 mixing ratio are also clearly correlated with deviations of CO and SF 6 mixing ratios. A three‐dimensional inverse model is employed in order to assist with the interpretation of observational data. In general, the model shows excellent agreement with the observed mean seasonal cycles of CH 4 , δ 13 C, and δD, including the observed phase behavior.
    Type of Medium: Online Resource
    ISSN: 0148-0227
    URL: Article
    DOI: 10.1029/1999JD901176
    Language: English
    Publisher: American Geophysical Union (AGU)
    Publication Date: 2000
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    Carbon 13 and D kinetic isotope effects in the reactions of CH 4 with O( 1 D ) and OH: New laboratory measurements and their implications for the isotopic composition of stratospheric methane
    American Geophysical Union (AGU) ; 2001
    In:  Journal of Geophysical Research: Atmospheres Vol. 106, No. D19 ( 2001-10-16), p. 23127-23138
    Details
    In: Journal of Geophysical Research: Atmospheres, American Geophysical Union (AGU), Vol. 106, No. D19 ( 2001-10-16), p. 23127-23138
    Abstract: Measurements of the 13 C and D kinetic isotope effects (KIE) in methane, 13C KIE = k ( 12 CH 4 )/ k ( 13 CH 4 ) and D KIE = k ( 12 CH 4 )/ k ( 12 CH 3 D), in the reactions of these atmospherically important methane isotopomers with O( 1 D) and OH have been undertaken using mass spectrometry and tunable diode laser absorption spectroscopy to determine isotopic composition. For the carbon kinetic isotope effect in the reaction with the OH radical, 13C KIE OH = 1.0039 (±0.0004, 2σ) was determined at 296 K, which is significantly smaller than the presently accepted value of 1.0054 (±0.0009, 2 σ). For D KIE OH we found 1.294 (± 0.018, 2σ) at 296 K, consistent with earlier observations. The carbon kinetic isotope effect in the reaction with O( 1 D ) 13C KIE O(1 D ) , was determined to be 1.013, whereas the deuterium kinetic isotope effect is given by D KIE O(1 D ) = 1.06. Both values are approximately independent of temperature between 223 and 295 K. The room temperature fractionation effect 1000(KIE‐1) in the reaction of O( 1 D ) with 12 CH 4 versus CH 4 is thus ≈ 13‰, which is an order of magnitude greater than the previous value of 1‰. In combination with recent results from our laboratory on 13C KIE and D KIE for the reaction of CH 4 with Cl, these new measurements were used to simulate the effective kinetic isotope effect for the stratosphere with a two‐dimensional, time dependent chemical transport model. The model results show reasonable agreement with field observations of the 13 CH 4 / 12 CH 4 ratio in the lowermost stratosphere, and also reproduce the observed CH 3 D/CH 4 ratio.
    Type of Medium: Online Resource
    ISSN: 0148-0227
    URL: Article
    DOI: 10.1029/2000JD000120
    Language: English
    Publisher: American Geophysical Union (AGU)
    Publication Date: 2001
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