Imaging the rotationally state-selected NO(A,n) product from the predissociation of the A state of the NO-Ar van der Waals cluster

W.G. Roeterdink, K.E. Strecker, C.C. Hayden, M.H.M. Janssen, D.W. Chandler

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    Abstract

    The origin of the resonant structures in the spectrum of the predissociative part of the A state in the NO-Ar van der Waals cluster has been investigated. We have employed direct excitation to the predissociative part of the NO-Ar A state followed by rotational state selective ionization of the NO fragment. Velocity map imaging of the NO ion yields the recoil energy of the rotational state-selected fragment. A substantial contribution of rotational hotbands to the resonant structures is observed. Our data indicate that a centrifugal barrier as the origin of these resonances can be ruled out. We hypothesize that after the NO-Ar cluster is excited to the A state sufficient mixing within the rotating cluster takes place as it changes geometry from being T shaped in the NO (X) -Ar state to linear in the NO (A) -Ar state. This mixing allows the low energy and high angular momentum (J≈4.5) tumbling motion of the initially populated hotbands in the ground state NO (X) -Ar complex to be converted into NO (A,n=2) spinning rotation in the A state of the complex. The electronically excited spinning complex falls apart adiabatically producing rotationally excited NO (A,n=2) at the energetic threshold. This interpretation indicates that the resonances can be attributed to some type of vibrational Feshbach resonance. The appearance energy for the formation of NO (A,n=0) +Ar is found to be 44294.3±1.4 cm-1. © 2009 American Institute of Physics.
    Original languageEnglish
    Pages (from-to)134305
    JournalJournal of Chemical Physics
    Volume130
    Issue number13
    DOIs
    Publication statusPublished - 2009

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