Monitoring Chemical Reactions with Terahertz Rotational Spectroscopy

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dc.citation.firstpage3097
dc.citation.issueNumber8
dc.citation.journalTitleACS Photonics
dc.citation.lastpage3106
dc.citation.volumeNumber5
dc.contributor.authorSwearer, Dayne F.
dc.contributor.authorGottheim, Samuel
dc.contributor.authorSimmons, Jay G.
dc.contributor.authorPhillips, Dane J.
dc.contributor.authorKale, Matthew J.
dc.contributor.authorMcClain, Michael J.
dc.contributor.authorChristopher, Phillip
dc.contributor.authorHalas, Naomi J.
dc.contributor.authorEveritt, Henry O.
dc.date.accessioned2018-11-09T14:59:56Z
dc.date.available2018-11-09T14:59:56Z
dc.date.issued2018
dc.description.abstractRotational spectroscopy is introduced as a new in situ method for monitoring gas-phase reactants and products during chemical reactions. Exploiting its unambiguous molecular recognition specificity and extraordinary detection sensitivity, rotational spectroscopy at terahertz frequencies was used to monitor the decomposition of carbonyl sulfide (OCS) over an aluminum nanocrystal (AlNC) plasmonic photocatalyst. The intrinsic surface oxide on AlNCs is discovered to have a large number of strongly basic sites that are effective for mediating OCS decomposition. Spectroscopic monitoring revealed two different photothermal decomposition pathways for OCS, depending on the absence or presence of H2O. The strength of rotational spectroscopy is witnessed through its ability to detect and distinguish isotopologues of the same mass from an unlabeled OCS precursor at concentrations of <1 nanomolar or partial pressures of <10 μTorr. These attributes recommend rotational spectroscopy as a compelling alternative for monitoring gas-phase chemical reactants and products in real time.
dc.identifier.citationSwearer, Dayne F., Gottheim, Samuel, Simmons, Jay G., et al.. "Monitoring Chemical Reactions with Terahertz Rotational Spectroscopy." <i>ACS Photonics,</i> 5, no. 8 (2018) American Chemical Society: 3097-3106. https://doi.org/10.1021/acsphotonics.8b00342.
dc.identifier.digitalChemicalReactions
dc.identifier.doihttps://doi.org/10.1021/acsphotonics.8b00342
dc.identifier.urihttps://hdl.handle.net/1911/103293
dc.language.isoeng
dc.publisherAmerican Chemical Society
dc.rightsThis is an open access article published under an ACS AuthorChoice License, which permits copying and redistribution of the article or any adaptations for non-commercial purposes.
dc.rights.urihttps://pubs.acs.org/page/policy/authorchoice_termsofuse.html
dc.subject.keywordaluminum nanocrystals
dc.subject.keywordcarbonyl sulfide
dc.subject.keywordphotocatalysis
dc.subject.keywordplasmonics
dc.subject.keywordrotational spectroscopy
dc.titleMonitoring Chemical Reactions with Terahertz Rotational Spectroscopy
dc.typeJournal article
dc.type.dcmiText
dc.type.publicationpublisher version
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