Abstract
The reported values of the nonlinear refractive index n(l) of CS2 near 10 μm differ by 3 orders of magnitude, and the mechanisms responsible for the nonlinearity are not understood.1 We measure n(l) for CS2 directly by observing the deflection of a CO2 laser beam which traverses a prismatic cell filled with CS2 as a function of intensity up to 10 MW/cm2 at different frequencies. At 10.6 μm ∂n/∂l is positive, while at 9.5 μm ∂n/∂l is negative. Based on our results and the known CS2 absorption and linear dispersion curves, we conclude that three mechanisms contribute to the nonlinearity: (1) the molecular reorientation Kerr effect resulting in frequency-independent relatively small positive n2 values1; (2) thermal effects with negative n2 responsible for self-defocusing; (3) near two-photon resonance with vibronic states2 at 6.7 and 4.7 μm. The sign of the third contribution to n(l) depends on which side of the corresponding resonance the 2vL frequency is situated, while its magnitude is proportional to the laser intensity squared.
© 1987 Optical Society of America
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