Resonant Infrared Third-Harmonic Generation in Cryogenic Liquids

Abstract

We have observed two-photon resonantly enhanced tripling of C${\mathrm{O}}_2$-laser radiation in liquid CO mixtures. Using a tight-focusing geometry, a power conversion efficiency of 0.3% for the C${\mathrm{O}}_2$ $R\left(6\right)\mathrm{}$ line at 1069.01 ${\mathrm{cm}}^{-1\mathrm{}}$ has been achieved for a CO-${\mathrm{O}}_2$ solution. The solvent dependence of the CO two-photon resonance has been studied. Phasematching with an additional molecular constituent has been demonstrated.