Nonlinear optical properties and crystal characteristics of carbohydrazono-pyrazole derivatives have been studied. Many hydrazone derivatives have been synthesized and their second-harmonic generation efficiencies have been screened by means of the powder technique. Among them, it is found that 1-methyl-4-nicotinic aldehydecarbohydrazono-5-aminopyrazole (MNACAP) has a large second-order nonlinear efficiency. The MNACAP crystal belongs to the space group P21. The nonlinear coefficient of crystalline MNACAP is predicted using X-ray diffraction results and the molecular hyperpolarizability derived from the molecular orbital theoretical calculation. It is also confirmed that MNACAP has a short cut-off wavelength around 390 nm and has the high melting point of 265°C.
The angularly phase-matched second-harmonic generation (SHG) in ferroelectric liquid crystal has been studied as a function of electric field strength, sample thickness, rotating angle and temperature. A sharp angular phase-matching curve of the SHG controlled by an electric field is observed even in the liquid crystal. The temperature dependence of the phase-matched SHG in the ferroelectric phase has also been studied, and the temperature-tuned phase matching of SHG is realized by using the change in tilt angle of the ferroelectric liquid crystal.
The profile of the phase-matching behavior of second-harmonic generation in ferroelectric liquid crystal has been found to be strongly dependent on cell thickness. A sharp angular phase-matching curve of the second-harmonic generation with the full width at half-maximum of ∼1° is observed even in the liquid crystal. The effective nonlinear optical coefficient d
eff at the phase-matching condition is determined. The temperature dependence of the phase-matching behavior in the ferroelectric phase has also been studied.
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