Abstract: | We demonstrate a theoretical model and the experimental proof of a new method for n(2) measurements using single pulses. The advantage of the method is fast measurement, a simple setup, and independence from small nonlinear absorptions and thermal effects. We report on first n(2) measurements with the new technique on carbon disulfide, toluene, and a polymer dissolved in toluene to demonstrate the measurement of positive and negative third-order nonlinearities. We achieved a sensitivity of greater than lambda/200 phase-front distortion using picosecond Nd:YLF laser pulses. The given theory shows that attainment of higher sensitivities is possible. |