Structure and predissociation of the 3p;uD3Σ u+ Rydberg state of N2: First extreme-ultraviolet and new near-infrared observations, with coupled-channels analysis

B. R. Lewis, K. G.H. Baldwin, A. N. Heays, S. T. Gibson, J. P. Sprengers, W. Ubachs, M. Fujitake

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    Abstract

    The 3p;uD3Σu+ Rydberg state of N2 is studied experimentally using two high-resolution spectroscopic techniques. First, the forbidden D 3 Σu+ -X1 Σg+ transition is observed for the first time via the (0,0) band of 14N 2 and the (1,0) band of 15N2, using 1 extreme-ultraviolet +1 ultraviolet two-photon-ionization laser spectroscopy. Second, the Rydberg-Rydberg transition D 3Σu+ -E 3Σ g+ is studied using near-infrared diode-laser photoabsorption spectroscopy, thus extending the previous measurements of Kanamori [J. Chem. Phys. 95, 80 (1991)], to higher transition energies, and thereby revealing the (2,2) and (3,3) bands. The combined results show that the D (v=0-3) levels exhibit rapidly increasing rotational predissociation as v increases, spanning nearly four orders of magnitude. The D -state level structure and rotational predissociation signature are explained by means of a coupled-channels model which considers the electrostatically coupled 3Πu Rydberg-valence manifold, together with a pure-precession L -uncoupling rotational interaction between the 3p;uD3Σu+ and 3p π u G 3Πu Rydberg p -complex components.

    Original languageEnglish
    Article number204303
    JournalJournal of Chemical Physics
    Volume129
    Issue number20
    DOIs
    Publication statusPublished - 2008

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