In terms of the model for Llano anilinium-vermiculte intercalate proposed in Part I of this series, (M. Raupach and L.J. Janik, J. Colloid Interface Sci. 121, 449 (1988)) mutual dipole induction and surface dipole image effects explain the detailed band structure and frequency shifts observed over two ranges (3750–2550 and 1590-1550 cm −1 of the infrafed spectrum. The induction effects were estimated from polarizabilities and the distance between the interacting dipoles. The polarizabilities depend on the composition and charge of the interacting groups. Sets of two and eight frequency shifts (∼30 cm −1) were associated with the interaction of NH with charged and uncharge (respectively) inner OH from the octahedral sheet of the clay. Two furthers sets of IR bands, cach having larger frequency shifts (∼230 cm −1), were related to the interaction of -NH 3 with water and to the interaction of NH with the charged surface oxygens of the clay. The NH bending modes gave an obvious split producing bands of differing polarization with respect to the clay surface. The magniture of this was estimated, using surface dipole images, from the interdiple distance of the adsorbate dipole units, their radius, the dipole-image distance, relevat dielectric constants, and the transverse optical phonon frequency of the adsorbate. The dipole images were found to be set up close to tetrahedral substitution sites in one vermiculite and somewhat toward the octahedral layer from those sites in a second vericulite. Transverse optical phonon frequencies were found to support the idea of resonance between the absorbate and the clay and hence Model 2 proposed in Part I.