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• W2897854954 abstract "In this paper, two levels of theory are developed to determine the role of scattering resonances in the process of ozone formation. At the lower theory level, we compute resonance lifetimes in the simplest possible way, by neglecting all couplings between the diabatic vibrational channels in the problem. This permits to determine the effect of “shape” resonances, trapped behind the centrifugal barrier and populated by quantum tunneling. At the next level of theory, we include couplings between the vibrational channels, which permits to determine the role of Feshbach resonances and interaction of different reaction pathways on the global PES of ozone. Pure shape resonances are found to contribute little to the overall recombination process since they occur rather infrequently in the spectrum, in the vicinity of the top of the centrifugal barrier only. Moreover, the associated isotope effects are found to disagree with experimental data. By contrast, Feshbach-type resonances are found to make dominant contribution to the process. They occur in a broader range of spectrum, and their density of states is much higher. The properties of Feshbach resonances are studied in detail. They explain the isotopic ζ-effect, giving theoretical prediction in good agreement with experiments for both singly and doubly substituted ozone molecules. Importantly, Feshbach resonances also contribute to the isotopic η-effect, moving theoretical predictions in the right direction. Some differences with experimental data remain, which indicates that there may be another additional source of the η-effect." @default.
• W2897854954 created "2018-10-26" @default.
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• W2897854954 date "2018-10-22" @default.
• W2897854954 modified "2023-10-03" @default.
• W2897854954 title "Several levels of theory for description of isotope effects in ozone: Effect of resonance lifetimes and channel couplings" @default.
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• W2897854954 doi "https://doi.org/10.1063/1.5042590" @default.
• W2897854954 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/30384731" @default.
• W2897854954 hasPublicationYear "2018" @default.
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