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dc.contributor.authorHarris, Eliza
dc.contributor.authorNelson, David D.
dc.contributor.authorZahniser, Mark
dc.contributor.authorMcManus, Barry J.
dc.contributor.authorPrinn, Ronald G.
dc.contributor.authorOno, Shuhei
dc.contributor.authorOlszewski, William J.
dc.contributor.authorPotter, Katherine Ellison
dc.contributor.authorWhitehill, Andrew Richard
dc.date.accessioned2014-12-22T17:27:28Z
dc.date.available2014-12-22T17:27:28Z
dc.date.issued2013-12
dc.date.submitted2013-10
dc.identifier.issn0003-2700
dc.identifier.issn1520-6882
dc.identifier.urihttp://hdl.handle.net/1721.1/92437
dc.description.abstractNitrous oxide is an important greenhouse gas and ozone-depleting-substance. Its sources are diffuse and poorly characterized, complicating efforts to understand anthropogenic impacts and develop mitigation policies. Online, spectroscopic analysis of N[subscript 2]O isotopic composition can provide continuous measurements at high time resolution, giving new insight into N[subscript 2]O sources, sinks, and chemistry. We present a new preconcentration unit, “Stheno II”, coupled to a tunable infrared laser direct absorption spectroscopy (TILDAS) instrument, to measure ambient-level variations in [superscript 18]O and site-specific [superscript 15]N N[subscript 2]O isotopic composition at remote sites with a temporal resolution of <1 h. Trapping of N[subscript 2]O is quantitative up to a sample size of ~4 L, with an optimal sample size of 1200–1800 mL at a sampling frequency of 28 min. Line shape variations with the partial pressure of the major matrix gases N[subscript 2]/O[subscript 2] and CO[subscript 2] are measured, and show that characterization of both pressure broadening and Dicke narrowing is necessary for an optimal spectral fit. Partial pressure variations of CO[subscript 2] and bath gas result in a linear isotopic measurement offset of 2.6–6.0 ‰ mbar[superscript –1]. Comparison of IR MS and TILDAS measurements shows that the TILDAS technique is accurate and precise, and less susceptible to interferences than IR MS measurements. Two weeks of measurements of N[subscript 2]O isotopic composition from Cambridge, MA, in May 2013 are presented. The measurements show significant short-term variability in N[subscript 2]O isotopic composition larger than the measurement precision, in response to meteorological parameters such as atmospheric pressure and temperature.en_US
dc.description.sponsorshipNational Science Foundation (U.S.) (Grant 0959280)en_US
dc.language.isoen_US
dc.publisherAmerican Chemical Society (ACS)en_US
dc.relation.isversionofhttp://dx.doi.org/10.1021/ac403606uen_US
dc.rightsArticle is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use.en_US
dc.sourceProf. Prinn via Chris Sherratten_US
dc.titleDevelopment of a Spectroscopic Technique for Continuous Online Monitoring of Oxygen and Site-Specific Nitrogen Isotopic Composition of Atmospheric Nitrous Oxideen_US
dc.typeArticleen_US
dc.identifier.citationHarris, Eliza, David D. Nelson, William Olszewski, Mark Zahniser, Katherine E. Potter, Barry J. McManus, Andrew Whitehill, Ronald G. Prinn, and Shuhei Ono. “Development of a Spectroscopic Technique for Continuous Online Monitoring of Oxygen and Site-Specific Nitrogen Isotopic Composition of Atmospheric Nitrous Oxide.” Analytical Chemistry 86, no. 3 (February 4, 2014): 1726–1734.en_US
dc.contributor.departmentMassachusetts Institute of Technology. Center for Global Change Scienceen_US
dc.contributor.departmentMassachusetts Institute of Technology. Department of Earth, Atmospheric, and Planetary Sciencesen_US
dc.contributor.approverPrinn, Ronald G.en_US
dc.contributor.mitauthorHarris, Elizaen_US
dc.contributor.mitauthorOlszewski, William J.en_US
dc.contributor.mitauthorPotter, Katherine Ellisonen_US
dc.contributor.mitauthorWhitehill, Andrew Richarden_US
dc.contributor.mitauthorPrinn, Ronald G.en_US
dc.contributor.mitauthorOno, Shuheien_US
dc.relation.journalAnalytical Chemistryen_US
dc.eprint.versionAuthor's final manuscripten_US
dc.type.urihttp://purl.org/eprint/type/JournalArticleen_US
eprint.statushttp://purl.org/eprint/status/PeerRevieweden_US
dspace.orderedauthorsHarris, Eliza; Nelson, David D.; Olszewski, William; Zahniser, Mark; Potter, Katherine E.; McManus, Barry J.; Whitehill, Andrew; Prinn, Ronald G.; Ono, Shuheien_US
dc.identifier.orcidhttps://orcid.org/0000-0001-5996-8217
dc.identifier.orcidhttps://orcid.org/0000-0001-5925-3801
dc.identifier.orcidhttps://orcid.org/0000-0002-1348-9584
mit.licensePUBLISHER_POLICYen_US
mit.metadata.statusComplete


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