Abstract

Presented here are the first results of experiments on multiple-photon excitation (MPE) of molecules upon their being concurrently irradiated by several IR pulses differing in frequency. Effective population of the high vibrational states (HVS) of SF6 was found to occur even when the frequencies of exciting pulses were fairly far (10–20 cm–1) from the linear absorption spectrum (LAS) of the molecules. The method enables one to obtain narrow vibrational distributions of excited molecules (VDEM) and make a wider use of the capabilities of IR lasers for selective photochemistry purposes.