Abstract. The phase-matched direct tripling of picosecond light pulses of a mode-locked Nd: glass laser in a new cyanine dye PMC is studied. The solvents trifluoroethanol (TFE) and hexafluoroisopropanol (HFIP) are applied. The S Q -S l absorption peak of the dye is around A = 480 nm and the absorption cross section at the third-harmonic wavelength of A 3 = 351.3 nm is only a 3 « 1 x 10~1 9 cm 2 . Phase-matching occurred at concentrations of C PM = 0.0874 mol/dm 3 in HFIP and 0.1088 mol/dm 3 in TFE. A third-harmonic energy conversion efficiency of r] E « 0.01 was achieved at a pump-laser peak intensity of I 0L « 2.5 x 10 11 W/cm 2 in a 5 mm long sample of PMC in TFE. The conversion efficiency is limited by destruction of phase-matching due to the intensity-dependent nonlinear refractive index of the dye solutions.
PACS: 42.65Efficient frequency tripling of laser radiation is performed generally in a two-step process first generating the secondharmonic light in a phase-matched nonlinear optical crystal and then frequency mixing the fundamental and the secondharmonic light in another phase-matched nonlinear optical crystal [1][2][3]. The second-order nonlinear optical susceptibility x ( 2 ) is responsible for these conversion processes. Direct (single-step) angle-tuned phase-matched third-harmonic generation of Nd:laser radiation was realized in the crystals LiI0 3 [4], CaC0 3 [5], and /3-BaB 2 0 4 [6]. In the vapor phase efficient phase-matched third-harmonic generation of Nd: laser radiation was achieved in mixtures of alkali vapors and noble gases [2,[7][8][9][10][11][12][13]. The direct third-harmonic generation is caused by the third-order nonlinear optical susceptibility x (3) .Phase-matched third-harmonic generation of Nd: laser radiation in organic dye solutions was studied in [14][15][16][17][18][19]. Dyes having the S 0 -S l absorption peak between the fundamental and third-harmonic frequency were selected for a low absorption cross section at the third-harmonic frequency. They were dissolved in a solvent of low normal refractive index dispersion. Phase-matching was achieved at a certain dye concentration at which the anomalous refractive index dispersion of the dyes compensated the normal refractive index dispersion of the solvents. For the dye PYC dissolved in hexafluoroisopropanol the absorption cross section at the third-harmonic frequency v 3 was cr 3 = 3.55 x 10~1 8 cm 2 , the two-photon absorption cross section was a^l = 1.8 x 10~4 9 cm 4 s and the excitedstate absorption cross section of third-harmonic light was a 3 e x = 2.6 x 10~1 6 cm 2 [18]. A maximum third-harmonic energy conversion efficiency of r] E = 2 x 10 -4 was achieved for input peak intensities J 0 L > 10 11 W/cm 2 (sample thickness I = 0.2 mm) [18]. The maximum obtainable conversion efficiency was limited by i) the small interaction length because of residual dye absorption at the third-harmonic frequency and ii) by two-photon dye absorption at twice the fundamental laser frequency and concomitant excited-state absorption of the dye....