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The phase-matched collinear third harmonic generation of picosecond laser pulses in a 0.0825 molar hexafluoroisopropanol solution of a pyrimidonecarbocyanine dye is studied. The fundamental pulses are generated in a passively mode-locked Nd-phosphate glass laser. The saturation of third harmonic generation at high intensities is investigated. The influences of two-photon absorption, excited-state absorption, and amplified spontaneous emission are discussed. For input peak intensities above 1011 W/cm2 a third harmonic energy conversion of about 2×10-4 is achieved.

Efficient phase-matched third harmonic light generation in hexafluoroisopropanol solutions of a pyrimidonecarbocyanine dye