Frequency-domain four-wave mixing (FD-4WM) spectroscopy is developed using an amplified Ti:sapphire laser as pump pulses and a Q-switched yttrium lithium fluoride laser locked to the Ti:sapphire laser as a probe. The diffracted beam is spectrally analyzed by a monochromator and detected by a charge coupled device camera. The signal obtained by this spectroscopy is expressed by the product of the square of the material response function and the second-order cross correlation function of the two pump pulses. We propose the following two applications of this spectroscopy: One is to obtain directly frequency information on the material response, which is difficult to obtain by means of usual homodyne-detected time-domain 4WM spectroscopy. The FD-4WM spectra obtained for liquid samples agree well with the results obtained by optically heterodyne-detected optical Kerr effect measurement. Besides, we have demonstrated the polarization-selected FD-4WM. The other application is the pulse diagnostic use of this spectroscopy: We have measured the FD-4WM spectra for a frequency-modulated pulse, a chirped pulse, and a frequency-modulated, linearly chirped pulse, and have demonstrated that the tempo-spectral relationship between the two pump pulses is very well expressed by the two-dimensional FD-4WM spectra.

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