Abstract
We study the dynamical effects of vibration-rotation coupling in multiple photon excitation at lowest order. Our molecular model is the simplest possible: that of an oscillator (triply degenerate) and uncoupled rigid rotor. The molecule-field interactions introduce a vibration-rotation nonlinearity which gives rise to nonconservation of the molecular angular momentum and in some instances consequent chaotic dynamics. The chaos leads to incoherence (widely seen in experiments1) in the time dependence of the photon absorption and is not treatable in an additive way as inhomogeneous broadening.2,4
Work perfrmed while on leave from the Physice Department, University of Arkansas, Fayetteville, Arkansas.
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Galbraith, H.W., Ackerhalt, J.R., Milonni, P.W. (1984). Chaos in a Semiclassical Model of Multiphoton Excitation of Spherical top Molecules. In: Mandel, L., Wolf, E. (eds) Coherence and Quantum Optics V. Springer, Boston, MA. https://doi.org/10.1007/978-1-4757-0605-5_104
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DOI: https://doi.org/10.1007/978-1-4757-0605-5_104
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