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We optimized the two-photon fluorescence (TPF) of a Coumarin 30 dye by using a feedback-controlled femtosecond pulse shaping technique. For optimization we implemented an evolutionary algorithm with a liquid crystal phase-only pulse shaper in a folded 4f setup. The optimization procedure applied to the second harmonic generation, and TPF noticeably improved the output signals and demonstrated good convergence. In addition, signal ratios involving TPF and second harmonic generation (SHG) were successfully optimized. The correlation between TPF and SHG was studied, and it was found to decrease when the pulse shape was close to the optimum. These experimental results are of interest for potential applications of coherent control to complex molecular systems as well as in biomedical imaging.

We study propagation of short laser pulses through water and use a spectral hole filling technique to essentially perform a sensitive balanced comparison of absorption coefficients for pulses of different duration. This study is motivated by an alleged violation of the Bouguer-Lambert-Beer law at low light intensities, where the pulse propagation is expected to be linear, and by a possible observation of femtosecond optical precursors in water. We find that at low intensities, absorption of laser light is determined solely by its spectrum and does not directly depend on the pulse duration, in agreement with our earlier work and in contradiction to some work of others. However, as the laser fluence is increased, interaction of light with water becomes nonlinear, causing energy exchange among the pulse's spectral components and resulting in peak-intensity dependent (and therefore pulse-duration dependent) transmission. For 30 fs pulses at 800 nm center wavelength, we determine the onset of nonlinear propagation effects to occur at a peak value of about 0.12 mJ/cm(2) of input laser energy fluence.