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• W2328554924 abstract "A new route for the nonradiative decay of photoexcited, H-bonded, nitrogen-containing, heterocyclic dimers is offered and exemplified by a study of the pyrazole dimer. In some of these systems the N(3s) Rydberg state is the lowest excited singlet state. This state is formed by direct light absorption or by nonradiative transition from the allowed ππ* state. An isomer of this Rydberg state is formed by H atom transfer to the other component of the dimer. The newly formed H-bonded radical pair is composed of two radicals (a H-adduct of pyrazole, a heterocyclic analogue of the NH4 radical) and the pyrazolium π-radical. It is calculated to have a shallow local minimum and is the lowest point on the PES of the H-pyrazole/pyrazolium radical pair. This species can cross back to the ground state of the original dimer through a relatively small energy gap and compete with the H-atom loss channel, known for the monomer. In both Rydberg dimers, an electron occupies a Rydberg orbital centered mostly on one of the two components of the dimer. This Rydberg Center Shift (RCS) mechanism, proposed earlier (Zilberg, S.; Kahan, A.; Haas, Y. Phys. Chem. Chem. Phys. 2012, 14, 8836), leads to deactivation of the electronically excited dimer while keeping it intact. It, thus, may explain the high photostability of the pyrazole dimer as well as other heterocyclic dimers." @default.
• W2328554924 created "2016-06-24" @default.
• W2328554924 creator A5054353824 @default.
• W2328554924 creator A5084222656 @default.
• W2328554924 date "2012-08-31" @default.
• W2328554924 modified "2023-09-25" @default.
• W2328554924 title "Role of Rydberg States in the Photostability of Heterocyclic Dimers: The Case of Pyrazole Dimer" @default.
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• W2328554924 doi "https://doi.org/10.1021/jp304325x" @default.
• W2328554924 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/22747495" @default.
• W2328554924 hasPublicationYear "2012" @default.
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