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Experimental and theoretical studies of the gas-phase reactions of O(1D) with H2O and D2O at low temperature

dc.contributor.authorHickson, Kevin
dc.contributor.authorBhowmick, Somnath
dc.contributor.authorSuleimanov, Yury
dc.contributor.authorBrandão, João
dc.contributor.authorCoelho, Daniela
dc.date.accessioned2022-02-15T12:03:18Z
dc.date.available2022-02-15T12:03:18Z
dc.date.issued2021-12-10
dc.description.abstractHere we report the results of an experimental and theoretical study of the gas-phase reactions between O($^1$D) and H$_2$O and O($^1$D) and D$_2$O at room temperature and below. On the experimental side, the kinetics of these reactions have been investigated over the 50-127 K range using a continuous flow Laval nozzle apparatus, coupled with pulsed laser photolysis and pulsed laser induced fluorescence for the production and detection of O($^1$D) atoms respectively. Experiments were also performed at 296 K in the absence of a Laval nozzle. On the theoretical side, the existing full-dimensional ground X$^1$A potential energy surface for the H$_2$O$_2$ system involved in this process has been reinvestigated and enhanced to provide a better description of the barrierless H-atom abstraction pathway. Based on this enhanced potential energy surface, quasiclassical trajectory calculations and ring polymer molecular dynamics simulations have been performed to obtain low temperature rate constants. The measured and calculated rate constants display similar behaviour above 100 K, showing little or no variation as a function of temperature. Below 100 K, the experimental rate constants increase dramatically, in contrast to the essentially temperature independent theoretical values. The possible origins of the divergence between experiment and theory at low temperatures are discussed.pt_PT
dc.description.sponsorshipK. M. H. acknowledges support from the French program ‘‘Physique et Chimie du Milieu Interstellaire’’ (PCMI) of the CNRS/INSU with the INC/INP co-funded by the CEA and CNES as well as funding from the ‘‘Programme National de Plane´tologie’’ (PNP) of the CNRS/INSU. This research was also supported by the EMME-CARE project that has received funding from the European Union’s Horizon 2020 Research and Innovation Program, under Grant Agreement No. 856612, as well as matching co-funding by the Government of the Republic of Cyprus. Y. V. S. was also supported by the Russian Foundation for Basic Research grant number 20-03-00833. S. B. acknowledges the financial support of the European Regional Development Fund and the Republic of Cyprus through the Research Promotion Foundation NANO2 LAB Project INFRASTRUCTURES/1216/0070. The RPMD computations have been performed on the ‘‘AMD EPYC’’ High Performance Computing Facility of The Cyprus Institute. J. B. and D. V. C. acknowledge the support by the FCT under the PTDC/QUI-QFI/31955/2017 research project, cofinanced by the European Community Fund, FEDER and the COST Action CA18212 ‘‘Molecular Dynamics in the GAS phase’’.pt_PT
dc.description.versioninfo:eu-repo/semantics/publishedVersionpt_PT
dc.identifier.doi10.1039/D1CP04614Dpt_PT
dc.identifier.issn1463-9076
dc.identifier.urihttp://hdl.handle.net/10400.1/17552
dc.language.isoengpt_PT
dc.peerreviewedyespt_PT
dc.publisherRoyal Society of Chemistrypt_PT
dc.relationEastern Mediterranean and Middle East – Climate and Atmosphere Research Centre
dc.titleExperimental and theoretical studies of the gas-phase reactions of O(1D) with H2O and D2O at low temperaturept_PT
dc.typejournal article
dspace.entity.typePublication
oaire.awardTitleEastern Mediterranean and Middle East – Climate and Atmosphere Research Centre
oaire.awardURIinfo:eu-repo/grantAgreement/EC/H2020/856612/EU
oaire.awardURIinfo:eu-repo/grantAgreement/FCT/9471 - RIDTI/PTDC%2FQUI-QFI%2F31955%2F2017/PT
oaire.citation.endPage25806pt_PT
oaire.citation.issue45pt_PT
oaire.citation.startPage25797pt_PT
oaire.citation.titlePhysical Chemistry Chemical Physicspt_PT
oaire.citation.volume23pt_PT
oaire.fundingStreamH2020
oaire.fundingStream9471 - RIDTI
person.familyNameBrandão
person.familyNameCoelho
person.givenNameJoão
person.givenNameDaniela
person.identifier.ciencia-id501B-3366-CB7B
person.identifier.orcid0000-0003-3047-7793
person.identifier.orcid0000-0001-7606-3479
person.identifier.ridA-6390-2010
person.identifier.scopus-author-id7004555284
project.funder.identifierhttp://doi.org/10.13039/501100008530
project.funder.identifierhttp://doi.org/10.13039/501100001871
project.funder.nameEuropean Commission
project.funder.nameFundação para a Ciência e a Tecnologia
rcaap.rightsrestrictedAccesspt_PT
rcaap.typearticlept_PT
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