Abstract

The predissociation rates of 600 vibrationally excited H 3 2sA 1 ′ states were obtained by three-dimensional wave packet calculations. Ab initio calculations were carried out for the nonadiabatic coupling matrix elements as well as a quantum defect surface of the H 3 2sA 1 ′ state, which were represented in terms of the hyperspherical coordinates to be utilized in the wave packet study. For the 2sA 1 ′ ground vibrational level, the estimated rate agrees well with the experimental value. The mean decay rate increases with vibrational energy, but the distribution largely scatters around the mean rate. An implication of the experiments for higher Rydberg states is given based on the analysis of the present results.

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