Abstract
We describe the results of a number of experiments which demonstrate competition between three-photon resonance-enhanced multiphoton ionisation and third-harmonic generation (THG) at wavelengths near the G̃ 1Π u-X̃ 1Σ g + (π u 3 4sσ g ← π u 4) Rydberg transition of acetylene. The results serve to strengthen a recent suggestion by Katz, Tsukiyama and Bersohn that THG will proveto be a general phenomenon for poly-atomic molecules with sharp Rydberg transitions.
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