Abstract
A picosecond IR laser pulse, pumping multiphoton resonance, can excite a molecule from the ground state to a certain high-lying vibrational level, all the other levels being unpopulated by the end of the pulse. The neighbouring multiphoton resonances do not overlap, though the power broadening required may be much greater than the intervals between them. Complete selective population of a specific vibrational level can be achieved only under certain conditions of laser pulse amplitude and duration. Based on this effect, a novel method for investigating vibrational energy intermolecular and intramolecular relaxation is proposed. The possibility of mode-selective multiphoton excitation of polyatomic molecules is discussed.
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