Most frequency-domain nonlinear-optical techniques measure only the magnitude of the Fourier transform of a temporal response and, hence, do not uniquely determine the response. We show that, for the commonly used response, h(t) = A exp(-t/τ_ƒ) + B exp(-t/τ_s),where A≡ α/τ_ƒ and B ≡ (1 - α)/τ_s, the spectral line shape can always be fitted by two different values of α. A measurement of the optical Kerr transient of carbon disulfide illustrates this ambiguitv. We also demonstrate a single-scan method that is free from such ambiguities. It involves adding coherent background with a nonzero quadrature-phase wavelength.

© 1988 Optical Society of America

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