Four-wave mixing in alkali halide crystals and aqueous solutions

Noncollinear phase-matched nonresonant four-photon frequency mixing _p+ _p– _{L s} in crystals and aqueous solutions of LiCl, CsCl, KF, and KI is studied. The concentration of the aqueous solutions is varied between 0.5 mol/l and saturation. Picosecond laser pulses of a mode-locked Nd-glass laser are applied as pump pulses. The energy conversion of laser light at frequency _L to frequency _S is measured and the nonlinear susceptibilities ⁽³⁾ are calculated. The dependence of the hyperpolarizabilities on concentration is analysed and gives information on the solute-solvent interaction.