High-intensity femtosecond pulses tunable in the 0.8–1.6-μm range have been generated by parametric amplification of a continuum white light in a new organic crystal, N-(4-nitrophenyl)-L-prolinol (NPP). The traditional concept of noncritical phase matching was revised in view of requirements linked to the observation of ultrafast subpicosecond nonlinear phenomena. The notions of θ (noncritical) and λ (noncritical) phase matching are introduced together with their applications. An experimental determination of phase-matching curves for both second-harmonic generation and three-wave mixing has been carried out. A θ noncritical phase-matching configuration for second-harmonic generation at 1.15 μm and a quasi-λ noncritical phase-matching configuration in the near IR for three-wave mixing were evidenced. Frequency and pump-intensity dependences of the gain have also been studied. Parametric emission at degeneracy was observed, with the emitted bandwidth extending from 1.0 to 1.4 μm. Time resolution of the amplified signal has been carried out by cross correlating the pump with the incoming signal, evidencing a reduced time broadening of the interacting pulses; a new spectroscopic method with subpicosecond time resolution is derived from the previous nonlinear optical characterization experiments by replacing the IR continuum from the water cell by any sample emitting in the same frequency range. This method, termed parametric amplification and sampling spectroscopy, was used for temporal analysis of amplified and emitted infrared signals generated in an NPP crystal.
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