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Nonadiabatic molecular dynamics study of a complete photoswitching cycle for a full-size diarylethene system

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cris.lastimport.scopus2024-02-12T19:45:02Z
dc.abstract.enDiarylethene (DAE) photoswitches continue to stay under the spotlight as remarkably stable, ultrafast, and efficient light-driven controlling units for applications in molecular technologies and devices. While tremendous amount of work has been put into rationalizing their performance, several fundamental questions about their switching mechanism remain. In this work, we undertake the challenge to provide, for the first time, the real-time theoretical description of a full-size DAE photoswitch operation dynamics, which becomes possible with employment of the cutting-edge multi-reference semi-empirical ODM2/MRCI methodology. To this end, we perform on-the-fly NAMD simulations of the cyclization and cycloreversion reaction for a flagship DAE system: 1,2-Bis(2-methyl-3-benzothienyl) perfluorocyclopentene, known as BT. Eventually, we obtain very good agreement of predicted photoswitching quantum yields with available experimental data, reporting the efficiency of the ring-opening and the efficiency of the ring-closure transformations, as compared to the 50% and 30% efficiencies, respectively, reported by Ishibashi et al. (J. Phys. Chem. C 2016, 120, 2, 1170–1177). On this grounds, we complement the existing view on the BT photoswitching with explicit predictions of the branching ratio at the reactive conical intersection, and by qualitative estimation of a side relaxation through quasi-degeneration seam. We believe that our results finally open prospects for future wide-range theoretical studies on DAE photoswitching, eventually providing researchers with a long-awaited tool to understand and control their operation.
dc.affiliationUniwersytet Warszawski
dc.contributor.authorJankowska, Joanna
dc.contributor.authorMartyka, Mikołaj
dc.date.accessioned2024-01-25T13:50:36Z
dc.date.available2024-01-25T13:50:36Z
dc.date.copyright2022-12-22
dc.date.issued2022
dc.description.accesstimeAT_PUBLICATION
dc.description.financePublikacja bezkosztowa
dc.description.versionFINAL_PUBLISHED
dc.description.volume438
dc.identifier.doi10.1016/J.JPHOTOCHEM.2022.114513
dc.identifier.issn1010-6030
dc.identifier.urihttps://repozytorium.uw.edu.pl//handle/item/113818
dc.identifier.weblinkhttps://api.elsevier.com/content/article/PII:S1010603022007365?httpAccept=text/xml
dc.languageeng
dc.pbn.affiliationchemical sciences
dc.relation.ispartofJournal of Photochemistry and Photobiology A: Chemistry
dc.relation.pages114513
dc.rightsCC-BY-NC-ND
dc.sciencecloudnosend
dc.subject.enDiarylethenes
dc.subject.enNonadiabatic molecular dynamics
dc.subject.enPhotoswitching mechanism
dc.subject.enSwitching bias
dc.subject.enSemi-empirical methods
dc.titleNonadiabatic molecular dynamics study of a complete photoswitching cycle for a full-size diarylethene system
dc.typeJournalArticle
dspace.entity.typePublication