We have determined the dispersion of three independent nonlinear optical susceptibilities, l<2 15 l, \d n l and ldf 33 l, for CdS and CdSe. Tunable dye lasers (0.73 to 1.0 Mm) were used. In spite of the large absorption at the second harmonic and/or fundamental wavelengths, Kleinman's relation (d n^d3i ) holds. The ratio id 33 /d dl l exhibits dispersion and deviates from Robinson's relation (ratio of 2). The relative phase angles between d 15 and d 31 and between d gl and <2 33 were measured at two wavelengths by a new reflection interference technique.A II-VI semiconductor with 6mm point group has three independent nonlinear optical coefficients, d 15 , d 319 and d 33 . x Several calculations 2 ' 3 have suggested that additional symmetries exist among the components of the d tensor. For a lossless and dispersionless crystal, Kleinman 2 predicted d 15 =d 31 . Robinson, 3 using symmetry properties of isolated AB 4 tetrahedra, further predicted d 33 = -2d 31 . More recent calculations, 4 ' 5 based on Phillips's dielectric theory of electronegativity, 6,7 have yielded similar relations among the components of the d tensor. Levine 5 * 8 has calculated both the absolute magnitudes and signs of the nonlinear optical coefficients. These are in excellent agreement with experiment. 9 Recently, numerous experiments 10 " 12 and theory 13,14 have considered the dispersion of the nonlinear optical coefficients of 43m crystals in the region where 2MOJ is strongly absorbed. However, none of the theoretical and experimental results have dealt with crystals of 6mm symmetry in the absorption region. This paper will present the dispersion measurements of Id 33 1, \d 15 /d 31 \, and \d 33 /d 31 \ in the range where the second-harmonic photon energy 2H(JO is near and much larger than the exciton energy gaps of CdS and CdSe. The relative phases among d 15 , d 3l , and d 33 will also be presented at several wavelengths. Dispersion measurements of d coefficients in 6mm crystals will enable one to test the generality of the additional symmetry relations in the d tensor.The experimental arrangement and apparatus used in this investigation have been reported previously. 12 The tunable dye lasers 15 (0.7 to 1.0 |im) were pumped by a Q-switched ruby laser. The second-harmonic photons generated by transmission from the quartz monitor 16 and generated by reflection from the sample under study were detected by two photo multipliers (EMI 963 5QD). The two photocurrent outputs were digitized by a gated electronic pulse integrator which had the capability of accumulating data from successive laser pulses. The CdS and CdSe single crystals were oriented with their a axes as the face normal and their c axes in the crystal face. Since the generation of reflected second harmonic requires careful crystal preparation, the crystal surfaces were polished with Linde C, A, and B abrasives in succession and were then mildly etched. 17 The quality of the crystal surface was judged in two ways. First, the crystal surface had to have good mirrorlike reflection....