The nonlinear refractive-index (n 2 ) spectrum of ZnSe near the band gap (Xgap -450 nm) at 77 K was measured for the first time to our knowledge by using self-bending of a pulsed laser beam. The maximum nonlinearity, n 2 -1.9 X 10-8 cm 2 /W, measured by us is anomalously large, which cannot be explained by conventional thermally induced band-gap shrinkage.ZnSe is one of the semiconductor materials with large nonlinear refractive index, An ideal case of SB occurs when a slab beam with a triangular spatial intensity profile, I(y), propagates through a Kerr-like nonlinear medium 9 "13"1 4 to form a light-induced prism. If the nonlinear component of the refractive index is n 2 I, where n 2 is the coefficient of nonlinearity, the beam will be self-deflected in the farfield region by the angle ONL, ONL = n 2 LIO/ao,where ao is the beam size, L is the thickness of the nonlinear medium, and Io is the laser peak intensity in the nonlinear medium. For our experiment parameters we showed using Ref. 13 that a typical value for the relative error due to the use of a right-triangular model instead of a realistic semi-Gaussian profile is less than 10%. Thus the spectral distribution of n 2 , n2(), can be directly obtained by measuring ONL at different laser wavelengths. The cw measurements of SB1 2 in sodium vapor showed good consistency with the theory. In our experiment we observed SB in bulk ZnSe over the range 446-460 nm, with a maximum n 2 as large as 1.9 X 10-8 cm 2 /W, and used it to make direct spectral measurement of n 2 in ZnSe. The SB method for measuring the spectrum n 2 (X) may present certain advantages over other rhethods. It requires (in principle) a single shot per data point (X) (although, owing to the lack of the detection equipment required for that, our measurements here were based on multishot averaging), whereas the Z-scan technique 4 ' 7 ' 8 inherently involves many shots and requires high mechanical and laser shot-to-shot stability. SB also allows one to measure n 2 directly with one laser beam, in contrast to the technique that uses two (pump and probe) laser beams,1 5 and the results for n 2 are obtained indirectly (by using the Kramers-Kronig transformation).Last, the sign of n 2 can be directly determined from the SB direction.The experimental setup is shown in Fig. 1. An 8-nsec pulsed dye laser was pumped with a frequencytripled Nd:YAG laser. The collimated beam radius (1/e 2 ) after lenses L 3 and L 4 was ct3.5 mm, and the radial spot size in the sample plane was ao -100 ,um (which was calculated by using all the measured parameters of the optical system). A razor blade (RB) was inserted into the collimated beam to form a semiGaussian intensity profile, which was then imaged onto the ZnSe sample. After passing through the ZnSe, the beam was collimated by positive lens L 6 . By measuring the displacement of the peak of the SB profile DNL, the SB angle is determined to be ONL DNL/L6. The samples were 500-ym-thick single-crystal ZnSe cut from the large (1 cm X 1 cm X 2 cm) ZnSe boules grown by the...