Dynamics associated with a quasiperiodically forced Morse oscillator: Application to molecular dissociation

Abstract

The dynamics associated with a quasiperiodically forced Morse oscillator is studied as a classical model for molecular dissociation under external quasiperiodic electromagnetic forcing. The forcing entails destruction of phase-space barriers, allowing escape from bounded to unbounded motion. In contrast to the ubiquitous Poincaré map reduction of a periodically forced system, we derive a sequence of nonautonomous maps from the quasiperiodically forced system. We obtain a global picture of the dynamics, i.e., of transport in phase space, using a sequence of time-dependent two-dimensional lobe structures derived from the invariant homoclinic tangle of a persisting invariant saddle-type torus in a Poincaré section of an associated autonomous system phase space. Transport is specified in terms of two-dimensional lobes mapping from one to another within the sequence of lobe structures, and this provides the framework for studying basic features of molecular dissociation in the context of classical phase-space trajectories. We obtain a precise criterion for discerning between bounded and unbounded motion in the context of the forced problem. We identify and measure analytically the flux associated with the transition between bounded and unbounded motion, and study dissociation rates for a variety of initial phase-space ensembles, such as an even or weighted distribution of points in phase space, or a distribution on a particular level set of the unperturbed Hamiltonian (corresponding to a quantum state). A double-phase-slice sampling method allows exact numerical computation of dissociation rates. We compare single- and two-frequency forcing. Infinite-time average flux is maximal in a particular single-frequency limit; however, lobe penetration of the level sets of the unperturbed Hamiltonian can be maximal in the two-frequency case. The variation of lobe areas in the two-frequency problem gives one added freedom to enhance or diminish aspects of phase-space transport on finite time scales for a fixed infinite-time average flux, and for both types of forcing the geometry of lobes is relevant. The chaotic nature of the dynamics is understood in terms of a traveling horseshoe map sequence.