Abstract
A method for determining the anharmonic potential constants k 122, k 322, and k 2222 of linear triatomic molecules is formulated. The calculation makes use of experimental rotational constants B v and vibrational term values G v of low-lying vibrational levels. The anharmonic (Fermi) interactions among the triad (10 00), (02 00), (00 01) are treated explicitly, but otherwise the calculation is based on the usual second-order theory. The method is applied to four molecules for which sufficiently accurate experimental data are available: N 2O, ClCN, BrCN, and OCS. The internal consistency of the calculation is not very satisfactory, which suggests that higher-order terms in the vibration-rotation Hamiltonian cannot be neglected. However, a set of anharmonic constants is obtained for each molecule which is felt to be more reliable than those previously published.
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