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

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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.
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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",
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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 -