N2O mole fraction and isotopic composition at Dübendorf, Switzerland, from 2014-2016

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Auteurs principaux: Harris, Eliza, Mohn, Joachim
Format: Dataset Open Access
Langue:en
Publié: PANGAEA 2016
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author Harris, Eliza
Mohn, Joachim
author_facet Harris, Eliza
Mohn, Joachim
collection Datos científicos de ciencias marinas y ambientales
contents The isotopic composition of atmospheric nitrous oxide (N2O) was measured semicontinuously, at ~35 min frequency in intermittent periods of 1-6 days over one and a half years, using preconcentration coupled to a quantum cascade laser spectrometer at the suburban site of Dübendorf, Switzerland. The achieved measurement repeatability was 0.08 per mil, 0.11 per mil, and 0.10 per mil for d18O, site preference, and d15Nbulk respectively, which is better than or equal to standard flask sampling-based isotope ratio mass spectrometry performance. The observed mean diurnal cycle reflected the buildup of N2O from isotopically light sources on an isotopically heavy tropospheric background. The measurements were used to determine the source isotopic composition, which varied significantly compared to chemical and meteorological parameters monitored at the site. FLEXPART-COSMO transport modeling in combination with modified Emissions Database for Global Atmospheric Research inventory emissions was used to model N2O mole fractions at the site. Additionally, isotopic signatures were estimated for different source categories using literature data and used to simulate N2O isotopic composition over the measurement period. The model was able to capture variability in N2O mole fraction well, but simulations of isotopic composition showed little agreement with observations. In particular, measured source isotopic composition exhibited one magnitude larger variability than simulated, clearly indicating that the range of isotopic source signatures estimated from literature significantly underestimates true variability of source signatures. Source d18O signature was found to be the most sensitive tracer for urban/industry versus agricultural N2O. d15Nbulk and site preference may provide more insight into microbial and chemical emission processes than partitioning of anthropogenic source categories.
format Dataset Open Access
id pangaea_https___doi_org_10_1594_PANGAEA_864305
institution PANGAEA
language en
publishDate 2016
publisher PANGAEA
record_format pangaea
spellingShingle N2O mole fraction and isotopic composition at Dübendorf, Switzerland, from 2014-2016
Harris, Eliza
Mohn, Joachim
DATE/TIME; Duebendorf_Empa; Nitrous oxide; Nitrous oxide, standard deviation; Preconcentration coupled to QCLAS; Site preference, N2O; Site preference, N2O, standard deviation; Switzerland; δ15N, gas; δ15N, standard deviation; δ18O, gas; δ18O, standard deviation
The isotopic composition of atmospheric nitrous oxide (N2O) was measured semicontinuously, at ~35 min frequency in intermittent periods of 1-6 days over one and a half years, using preconcentration coupled to a quantum cascade laser spectrometer at the suburban site of Dübendorf, Switzerland. The achieved measurement repeatability was 0.08 per mil, 0.11 per mil, and 0.10 per mil for d18O, site preference, and d15Nbulk respectively, which is better than or equal to standard flask sampling-based isotope ratio mass spectrometry performance. The observed mean diurnal cycle reflected the buildup of N2O from isotopically light sources on an isotopically heavy tropospheric background. The measurements were used to determine the source isotopic composition, which varied significantly compared to chemical and meteorological parameters monitored at the site. FLEXPART-COSMO transport modeling in combination with modified Emissions Database for Global Atmospheric Research inventory emissions was used to model N2O mole fractions at the site. Additionally, isotopic signatures were estimated for different source categories using literature data and used to simulate N2O isotopic composition over the measurement period. The model was able to capture variability in N2O mole fraction well, but simulations of isotopic composition showed little agreement with observations. In particular, measured source isotopic composition exhibited one magnitude larger variability than simulated, clearly indicating that the range of isotopic source signatures estimated from literature significantly underestimates true variability of source signatures. Source d18O signature was found to be the most sensitive tracer for urban/industry versus agricultural N2O. d15Nbulk and site preference may provide more insight into microbial and chemical emission processes than partitioning of anthropogenic source categories.
title N2O mole fraction and isotopic composition at Dübendorf, Switzerland, from 2014-2016
topic DATE/TIME; Duebendorf_Empa; Nitrous oxide; Nitrous oxide, standard deviation; Preconcentration coupled to QCLAS; Site preference, N2O; Site preference, N2O, standard deviation; Switzerland; δ15N, gas; δ15N, standard deviation; δ18O, gas; δ18O, standard deviation
url https://doi.org/10.1594/PANGAEA.864305