The spectral and temporal characteristics and optical-conversion efficiency of laser pulses at 400 nm generated by second-harmonic generation (SHG) of a regeneratively amplified mode-locked Ti:sapphire laser were investigated both theoretically and experimentally. The theoretical investigation was done by taking into account cubic nonlinearity, pulse walk-off, group-velocity dispersion, Kerr nonlinearity, quadratic broadening, frequency chirping of the fundamental pulse, and higher-order nonlinear mixing such as backconversion and optical parametric processing. The experimental studies of the effects of crystal length and pumping intensity on the pulse duration, the spectrum, and the optical-conversion efficiency of the SHG were carried out in BBO and LBO crystals of various thicknesses and compared with the theory. It was found that in a non-transform-limited pulse, the most significant contribution to the temporal and spectral distortion of the SHG pulses is mainly due to the chirping of the fundamental beam and self-phase modulation at high pumping intensity and long crystal length. The optimum crystal length and pumping intensity for obtaining a high optical-conversion efficiency and a pure spectrum in SHG are also calculated and experimentally investigated. It was found that a transform-limited fundamental pulse is essential to obtain a high conversion efficiency and to preserve the temporal profile of the second-harmonic pulse. It is also found that for a non-transform-limited pulse, a 0.5–0.6-mm BBO crystal and a modest pumping intensity of are the most suitable for SHG.
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