Degenerate four-wave mixing (DFWM) spectroscopy is modified to exploit femtosecond pulses, phase-sensitive-detection, frequency (wavelength) agility, two-color (nearly degenerate multiwave mixing) radiation, and improved signal-to-noise capabilities that can be realized through a combination of new solid state lasers, nonlinear optical components, and novel design concepts. The resulting time-resolved nonlinear optical techniques permit “instantaneous” optical nonlinearities, such as two-photon absorption cross sections, to be accurately measured over the spectral range from 450 to 2500 nm (and with significantly greater effort from 225 to 5000 nm). The power of the new techniques is illustrated by their application to the definition of Hg two-photon resonances of C60 and C70 as well as to the characterization of optical nonlinearities in two linear chromophores of putative utility for sensor protection and electrooptic modulation. Explicitly, these measurements provide accurate determination of both transition energies and transition moments (matrix elements connecting the two photon levels). Results are compared to those previously reported in the literature illustrating the advantages and problems associated with particular measurement techniques. All of the molecules studied are found to exhibit two-photon absorption coefficients comparable to that of GaAs, the most studied putative sensor protection material (based on utilization of electronic optical nonlinearity). Femtosecond pulse techniques are shown, in all cases, to be necessary to avoid complications arising from excited-state absorption and relaxation phenomena. The importance of phase-sensitive detection in identifying complications from overlapping transitions is illustrated.