Predissociation mechanism for the lowest 1Π u states of N 2

B. R. Lewis*, S. T. Gibson, W. Zhang, H. Lefebvre-Brion, J. M. Robbe

*Corresponding author for this work

    Research output: Contribution to journalArticlepeer-review

    87 Citations (Scopus)

    Abstract

    Separate coupled-channel Schrödinger-equation (CSE) models of the interacting 1Π u (b,c,o) and 3Π u (C, C′) states of N2 are combined, through the inclusion of spin-orbit interactions, to produce a five-channel CSE model of the N2 predissociation. Comparison of the model calculations with an experimental database, consisting principally of detailed new measurements of the vibrational and isotopic dependence of the 1Π u linewidths and lifetimes, provides convincing evidence that the predissociation of the lowest 1Π u levels in N2 is primarily an indirect process, involving spin-orbit coupling between the b 1Π u - and C 3Π u -state levels, the latter levels themselves heavily predissociated electrostatically by the C′ 3Π u continuum. The well-known large width of the b (v=3) level in N214 is caused by an accidental degeneracy with C (v=9). This CSE model provides the first quantitative explanation of the predissociation mechanism for the dipole-accessible 1Π u states of N2, and is thus likely to prove useful in the construction of realistic radiative-transfer and photochemical models for nitrogen-rich planetary atmospheres.

    Original languageEnglish
    Article number144302
    JournalJournal of Chemical Physics
    Volume122
    Issue number14
    DOIs
    Publication statusPublished - 2005

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