Multiphoton processes in molecular gases

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Abstract
The availability of reliable, high-powered, pulsed, tunablc dyc lasers has opened the way to study of a whole host of multiphoton phenomena in molecular gases. This article opens with an overview of the enormous contributions that resonant multiphoton excitation methods are making to our knowledge of the spectroscopy and the dynamics of electronically excited molecules. Another well known class of ‘multiphoton phenomenon’ is exemplified by the various frequency up-conversion schemes now in existence—schemes in which, through use of a suitable nonlinear medium, two or more photons (of the same or different frequencies) may be combined to yield high-energy photons. We conclude this review by considering the potential of molecular gases as nonlinear media for the generation of useful intensities of narrow-bandwidth vacuum-ultraviolet radiation.