Abstract
Theoretical efficiency limitations for a two-photon resonant third-harmonic generation (THG) process are analyzed in a treatment which includes all nonlinear processes associated with the two-photon resonance assuming negligible material excitation. Results are presented for both collimated-beam and tight-focusing geometries. The theory is applied to experimental results for THG of CO <inf xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</inf> laser radiation in liquid CO-O <inf xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</inf> mixtures; good agreement is found for the observed saturation in the THG efficiency in a tight-focusing geometry.
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