Abstract
The algebraic resonance quantization (ARQ) method has previously been investigated for coupled Morse oscillators with moderate coupling and a substantial degree of classical chaos. This method is investigated here for strong coupling with the transition to global chaos and a Wigner distribution of level spacings in the quantum spectrum. A sparse matrix multiresonance approximation (SMRA) is found to give good results even when there is global chaos. A truncated basis set approximation (TMRA) is successful for moderate coupling but breaks down for strong coupling. Implications of these results for calculation of rotation–vibration levels of polyatomics in the regime of global chaos are discussed. Prospects for nonlinear least-squares fitting of experimental spectra in the regime of global chaos are also discussed.
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