EFFICIENT MOLECULAR DISSOCIATION BY A CHIRPED ULTRASHORT INFRARED-LASER PULSE

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 (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. © 1990 The American Physical Society.