Novel laser spectroscopic technique for continuous analysis of N2O isotopomers: Application and intercomparison with isotope ratio mass spectrometry

Jan Reent Köster (Corresponding Author), Reinhard Well, Béla Tuzson, Roland Bol, Klaus Dittert, Anette Giesemann, Lukas Emmenegger, Albert Manninen, Laura Cárdenas, Joachim Mohn

    Research output: Contribution to journalArticleScientificpeer-review

    34 Citations (Scopus)

    Abstract

    RATIONALE
    Nitrous oxide (N2O), a highly climate‐relevant trace gas, is mainly derived from microbial denitrification and nitrification processes in soils. Apportioning N2O to these source processes is a challenging task, but better understanding of the processes is required to improve mitigation strategies. The N2O site‐specific 15 N signatures from denitrification and nitrification have been shown to be clearly different, making this signature a potential tool for N2O source identification. We have applied for the first time quantum cascade laser absorption spectroscopy (QCLAS) for the continuous analysis of the intramolecular 15 N distribution of soil‐derived N2O and compared this with state‐of‐the‐art isotope ratio mass spectrometry (IRMS).

    METHODS
    Soil was amended with nitrate and sucrose and incubated in a laboratory setup. The N2O release was quantified by FTIR spectroscopy, while the N2O intramolecular 15 N distribution was continuously analyzed by online QCLAS at 1 Hz resolution. The QCLAS results on time‐integrating flask samples were compared with those from the IRMS analysis.

    RESULTS
    The analytical precision (2σ) of QCLAS was around 0.3 ‰ for the δ15Nbulk and the 15 N site preference (SP) for 1‐min average values. Comparing the two techniques on flask samples, excellent agreement (R2 = 0.99; offset of 1.2 ‰) was observed for the δ15Nbulk values while for the SP values the correlation was less good (R2 = 0.76; offset of 0.9 ‰), presumably due to the lower precision of the IRMS SP measurements.

    CONCLUSIONS
    These findings validate QCLAS as a viable alternative technique with even higher precision than state‐of‐the‐art IRMS. Thus, laser spectroscopy has the potential to contribute significantly to a better understanding of N turnover in soils, which is crucial for advancing strategies to mitigate emissions of this efficient greenhouse gas.
    Original languageEnglish
    Pages (from-to)216-222
    Number of pages6
    JournalRapid Communications in Mass Spectrometry
    Volume27
    Issue number1
    DOIs
    Publication statusPublished - 2013
    MoE publication typeA1 Journal article-refereed

    Fingerprint

    Laser spectroscopy
    Quantum cascade lasers
    Isotopes
    Mass spectrometry
    Absorption spectroscopy
    Lasers
    Nitrification
    Denitrification
    Soils
    Nitrous Oxide
    Greenhouse gases
    Nitrates
    Sucrose
    Gases
    Spectroscopy

    Keywords

    • laser spectroscopy
    • nitrous oxide

    Cite this

    Köster, Jan Reent ; Well, Reinhard ; Tuzson, Béla ; Bol, Roland ; Dittert, Klaus ; Giesemann, Anette ; Emmenegger, Lukas ; Manninen, Albert ; Cárdenas, Laura ; Mohn, Joachim. / Novel laser spectroscopic technique for continuous analysis of N2O isotopomers : Application and intercomparison with isotope ratio mass spectrometry. In: Rapid Communications in Mass Spectrometry. 2013 ; Vol. 27, No. 1. pp. 216-222.
    @article{7cd0e283e83d4ccab5ad1ff058ab982d,
    title = "Novel laser spectroscopic technique for continuous analysis of N2O isotopomers: Application and intercomparison with isotope ratio mass spectrometry",
    abstract = "RATIONALE Nitrous oxide (N2O), a highly climate‐relevant trace gas, is mainly derived from microbial denitrification and nitrification processes in soils. Apportioning N2O to these source processes is a challenging task, but better understanding of the processes is required to improve mitigation strategies. The N2O site‐specific 15 N signatures from denitrification and nitrification have been shown to be clearly different, making this signature a potential tool for N2O source identification. We have applied for the first time quantum cascade laser absorption spectroscopy (QCLAS) for the continuous analysis of the intramolecular 15 N distribution of soil‐derived N2O and compared this with state‐of‐the‐art isotope ratio mass spectrometry (IRMS).METHODSSoil was amended with nitrate and sucrose and incubated in a laboratory setup. The N2O release was quantified by FTIR spectroscopy, while the N2O intramolecular 15 N distribution was continuously analyzed by online QCLAS at 1 Hz resolution. The QCLAS results on time‐integrating flask samples were compared with those from the IRMS analysis.RESULTSThe analytical precision (2σ) of QCLAS was around 0.3 ‰ for the δ15Nbulk and the 15 N site preference (SP) for 1‐min average values. Comparing the two techniques on flask samples, excellent agreement (R2 = 0.99; offset of 1.2 ‰) was observed for the δ15Nbulk values while for the SP values the correlation was less good (R2 = 0.76; offset of 0.9 ‰), presumably due to the lower precision of the IRMS SP measurements.CONCLUSIONSThese findings validate QCLAS as a viable alternative technique with even higher precision than state‐of‐the‐art IRMS. Thus, laser spectroscopy has the potential to contribute significantly to a better understanding of N turnover in soils, which is crucial for advancing strategies to mitigate emissions of this efficient greenhouse gas.",
    keywords = "laser spectroscopy, nitrous oxide",
    author = "K{\"o}ster, {Jan Reent} and Reinhard Well and B{\'e}la Tuzson and Roland Bol and Klaus Dittert and Anette Giesemann and Lukas Emmenegger and Albert Manninen and Laura C{\'a}rdenas and Joachim Mohn",
    year = "2013",
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    pages = "216--222",
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    Köster, JR, Well, R, Tuzson, B, Bol, R, Dittert, K, Giesemann, A, Emmenegger, L, Manninen, A, Cárdenas, L & Mohn, J 2013, 'Novel laser spectroscopic technique for continuous analysis of N2O isotopomers: Application and intercomparison with isotope ratio mass spectrometry', Rapid Communications in Mass Spectrometry, vol. 27, no. 1, pp. 216-222. https://doi.org/10.1002/rcm.6434

    Novel laser spectroscopic technique for continuous analysis of N2O isotopomers : Application and intercomparison with isotope ratio mass spectrometry. / Köster, Jan Reent (Corresponding Author); Well, Reinhard; Tuzson, Béla; Bol, Roland; Dittert, Klaus; Giesemann, Anette; Emmenegger, Lukas; Manninen, Albert; Cárdenas, Laura; Mohn, Joachim.

    In: Rapid Communications in Mass Spectrometry, Vol. 27, No. 1, 2013, p. 216-222.

    Research output: Contribution to journalArticleScientificpeer-review

    TY - JOUR

    T1 - Novel laser spectroscopic technique for continuous analysis of N2O isotopomers

    T2 - Application and intercomparison with isotope ratio mass spectrometry

    AU - Köster, Jan Reent

    AU - Well, Reinhard

    AU - Tuzson, Béla

    AU - Bol, Roland

    AU - Dittert, Klaus

    AU - Giesemann, Anette

    AU - Emmenegger, Lukas

    AU - Manninen, Albert

    AU - Cárdenas, Laura

    AU - Mohn, Joachim

    PY - 2013

    Y1 - 2013

    N2 - RATIONALE Nitrous oxide (N2O), a highly climate‐relevant trace gas, is mainly derived from microbial denitrification and nitrification processes in soils. Apportioning N2O to these source processes is a challenging task, but better understanding of the processes is required to improve mitigation strategies. The N2O site‐specific 15 N signatures from denitrification and nitrification have been shown to be clearly different, making this signature a potential tool for N2O source identification. We have applied for the first time quantum cascade laser absorption spectroscopy (QCLAS) for the continuous analysis of the intramolecular 15 N distribution of soil‐derived N2O and compared this with state‐of‐the‐art isotope ratio mass spectrometry (IRMS).METHODSSoil was amended with nitrate and sucrose and incubated in a laboratory setup. The N2O release was quantified by FTIR spectroscopy, while the N2O intramolecular 15 N distribution was continuously analyzed by online QCLAS at 1 Hz resolution. The QCLAS results on time‐integrating flask samples were compared with those from the IRMS analysis.RESULTSThe analytical precision (2σ) of QCLAS was around 0.3 ‰ for the δ15Nbulk and the 15 N site preference (SP) for 1‐min average values. Comparing the two techniques on flask samples, excellent agreement (R2 = 0.99; offset of 1.2 ‰) was observed for the δ15Nbulk values while for the SP values the correlation was less good (R2 = 0.76; offset of 0.9 ‰), presumably due to the lower precision of the IRMS SP measurements.CONCLUSIONSThese findings validate QCLAS as a viable alternative technique with even higher precision than state‐of‐the‐art IRMS. Thus, laser spectroscopy has the potential to contribute significantly to a better understanding of N turnover in soils, which is crucial for advancing strategies to mitigate emissions of this efficient greenhouse gas.

    AB - RATIONALE Nitrous oxide (N2O), a highly climate‐relevant trace gas, is mainly derived from microbial denitrification and nitrification processes in soils. Apportioning N2O to these source processes is a challenging task, but better understanding of the processes is required to improve mitigation strategies. The N2O site‐specific 15 N signatures from denitrification and nitrification have been shown to be clearly different, making this signature a potential tool for N2O source identification. We have applied for the first time quantum cascade laser absorption spectroscopy (QCLAS) for the continuous analysis of the intramolecular 15 N distribution of soil‐derived N2O and compared this with state‐of‐the‐art isotope ratio mass spectrometry (IRMS).METHODSSoil was amended with nitrate and sucrose and incubated in a laboratory setup. The N2O release was quantified by FTIR spectroscopy, while the N2O intramolecular 15 N distribution was continuously analyzed by online QCLAS at 1 Hz resolution. The QCLAS results on time‐integrating flask samples were compared with those from the IRMS analysis.RESULTSThe analytical precision (2σ) of QCLAS was around 0.3 ‰ for the δ15Nbulk and the 15 N site preference (SP) for 1‐min average values. Comparing the two techniques on flask samples, excellent agreement (R2 = 0.99; offset of 1.2 ‰) was observed for the δ15Nbulk values while for the SP values the correlation was less good (R2 = 0.76; offset of 0.9 ‰), presumably due to the lower precision of the IRMS SP measurements.CONCLUSIONSThese findings validate QCLAS as a viable alternative technique with even higher precision than state‐of‐the‐art IRMS. Thus, laser spectroscopy has the potential to contribute significantly to a better understanding of N turnover in soils, which is crucial for advancing strategies to mitigate emissions of this efficient greenhouse gas.

    KW - laser spectroscopy

    KW - nitrous oxide

    U2 - 10.1002/rcm.6434

    DO - 10.1002/rcm.6434

    M3 - Article

    VL - 27

    SP - 216

    EP - 222

    JO - Rapid Communications in Mass Spectrometry

    JF - Rapid Communications in Mass Spectrometry

    SN - 0951-4198

    IS - 1

    ER -