Phase-matched third-harmonic generation in dye solutions

Various dyes are investigated for their capability of generating 3^rd harmonic of Nd-laser light. The feasibility of achieving phase matching is demonstrated by direct measurements of the index of refraction. Third-harmonic conversion of hexamethylindocarbocyanine iodide, diethyloxacarbocyanine iodide and fuchsin red are compared. The highest conversion is obtained for hexamethylindocarbocyanine iodide (80 times higher than in fuchsin red). A further enhancement of the third harmonic by a factor of 70 is expected for the fundamental laser light at 1.15 μm.