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Dissociation probabilities and populations of excited vibrational states are calculated numerically for interaction of a Morse oscillator with a chirped, ultrashort (tₚ{10}^{{{-}}11}$ sec), intense laser pulse. It is shown that if the pulse frequency {ω}(t) decreases at a specific rate adapted to the molecular anharmonicity, the dissociation probability is many orders of magnitude higher than for a monochromatic pulse of the same intensity. Such pulses should be useful for more efficient multiphoton dissociation of molecular bonds.
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Chelkowski et al. (1990) studied this question.
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