Publication
Experimental and theoretical studies of the gas-phase reactions of O(1D) with H2O and D2O at low temperature
dc.contributor.author | Hickson, Kevin | |
dc.contributor.author | Bhowmick, Somnath | |
dc.contributor.author | Suleimanov, Yury | |
dc.contributor.author | Brandão, João | |
dc.contributor.author | Coelho, Daniela | |
dc.date.accessioned | 2022-02-15T12:03:18Z | |
dc.date.available | 2022-02-15T12:03:18Z | |
dc.date.issued | 2021-12-10 | |
dc.description.abstract | Here 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.sponsorship | K. 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.version | info:eu-repo/semantics/publishedVersion | pt_PT |
dc.identifier.doi | 10.1039/D1CP04614D | pt_PT |
dc.identifier.issn | 1463-9076 | |
dc.identifier.uri | http://hdl.handle.net/10400.1/17552 | |
dc.language.iso | eng | pt_PT |
dc.peerreviewed | yes | pt_PT |
dc.publisher | Royal Society of Chemistry | pt_PT |
dc.relation | Eastern Mediterranean and Middle East – Climate and Atmosphere Research Centre | |
dc.title | Experimental and theoretical studies of the gas-phase reactions of O(1D) with H2O and D2O at low temperature | pt_PT |
dc.type | journal article | |
dspace.entity.type | Publication | |
oaire.awardTitle | Eastern Mediterranean and Middle East – Climate and Atmosphere Research Centre | |
oaire.awardURI | info:eu-repo/grantAgreement/EC/H2020/856612/EU | |
oaire.awardURI | info:eu-repo/grantAgreement/FCT/9471 - RIDTI/PTDC%2FQUI-QFI%2F31955%2F2017/PT | |
oaire.citation.endPage | 25806 | pt_PT |
oaire.citation.issue | 45 | pt_PT |
oaire.citation.startPage | 25797 | pt_PT |
oaire.citation.title | Physical Chemistry Chemical Physics | pt_PT |
oaire.citation.volume | 23 | pt_PT |
oaire.fundingStream | H2020 | |
oaire.fundingStream | 9471 - RIDTI | |
person.familyName | Brandão | |
person.familyName | Coelho | |
person.givenName | João | |
person.givenName | Daniela | |
person.identifier.ciencia-id | 501B-3366-CB7B | |
person.identifier.orcid | 0000-0003-3047-7793 | |
person.identifier.orcid | 0000-0001-7606-3479 | |
person.identifier.rid | A-6390-2010 | |
person.identifier.scopus-author-id | 7004555284 | |
project.funder.identifier | http://doi.org/10.13039/501100008530 | |
project.funder.identifier | http://doi.org/10.13039/501100001871 | |
project.funder.name | European Commission | |
project.funder.name | Fundação para a Ciência e a Tecnologia | |
rcaap.rights | restrictedAccess | pt_PT |
rcaap.type | article | pt_PT |
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