The optical properties of oriented montmorillonite aggregates were measured in both non-complexing and complexing media. The changes observed lead to the following conclusions. Preparing oriented aggregates of clays for optical examination requires considerable care to avoid spurious orientation effects. In determining the optical constants of montmorillonite aggregates the medium must wet and enter the aggregate readily and displace the air, particularly from the smaller pores, otherwise large form birefringence effects of uncertain magnitude will occur. A suitable medium is likely to be one that complexes montmorillonite. The complex it forms must have relatively isotropic interlamellar layers and this is more likely with isodimensional molecules. Consideration of complexes with simple compounds suggests that the intrinsic birefringence of aggregates is overestimated by conventional techniques.

Forming complexes with aromatic compounds usually results in the birefringence of the aggregate being essentially determined by the orientation and anisotropy of the intercalated molecules.