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The second-order nonlinear-optical response of a material is measured in two dimensions of frequency. This new spectroscopy technique, based on the use of Fourier-transform spectral interferometry, is a transposition to optics of two-dimensional nuclear magnetic resonance. Although we demonstrate the technique by measuring the second-order phase-matching map of a nonresonant nonlinear crystal, this method should find useful applications in the measurement of second-order nonlinear susceptibility and in photon-echo experiments.
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Lepetit et al. (1996) studied this question.
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