Previous studies of the defect structure of kaolinite have examined samples having a restricted level of defects. This study examined nine kaolinite samples having a large diversity of defect contents, as indicated by Hinckley indexes ranging from 1.44 to 0.18. The samples were chosen so as to cover this range in as regular a manner as possible. The types and abundances of the defects were determined by examining the X-ray powder diffraction profiles for the 02,11 and 20,13 bands. The diffraction intensities were measured by counting for a fixed time in steps of 0.01°2θ. Analysis of these diffraction profiles indicated that (1) the major defect is the existence of a translation between adjacent layers, which is not the usual (approximately a/3), but is related to that translation by the pseudo-mirror plane coincident with the long diagonal of the unit cell; (2) the existence of a few C layers among the B layer stacking is a minor defect; (3) many of the samples could be accurately modeled only by assuming the existence of two kaolinite phases; (4) the existence of only a few C layers in some samples does not support the idea of a continuous series from kaolinite to dickite through disordered intermediates; and (5) the Hinckley indexes of several samples depend on the relative proportions of the two types of kaolinite in the mixture.

The nine kaolinite samples fall into three groups: those having a low to moderate abundance of defects (Hinckley index > 0.43) are mixtures of two types of kaolinite (one almost free of defects, the other richer in defects); those having low Hinckley indexes (0.43 to 0.18) are single phases with different proportions of defects; and those which contain a single type of kaolinite, unlike the others in the nature of the interlayer translations and the greater abundance of C layers. The agreement between calculated and observed X-ray diffraction profiles is excellent for all specimens, except one sample (from Charentes) for which the fit is acceptable but not perfect.

Use of a discriminant analysis has verified and grouped three suspected varieties of kaolinite found in kaolin-rich clay strata of late Paleocene to early Eocene age across north-central Mississippi. Initial identification of each type of kaolinite was based on clay-texture characteristics observed on scanning electron micrographs and the differences in pattern configurations of X-ray diffractograms. The discriminant function used for data treatment clearly segregated and grouped each variety. The discrimination variables were found to be the Hinckley index and, to a lesser extent, the Si4+ content relative to the Al3+ content.

The oldest variety is the Blue Mountain clay, composed of preserved hexagonal plates usually clustered into booklets with a vermiform texture. The Ashland variety, stratigraphically younger than the Blue Mountain clay, appears to have been derived from the erosion of the Blue Mountain clay. The Ashland cannot be recognized by any type of diagnostic texture, as it is made up of individual plates that have been corroded and abraded to the point where a hexagonal outline can no longer be recognized. The Sardis variety is the stratigraphically youngest of the three varieties and is at least a second, or possibly a third generation detrital product. The Sardis clay can be recognized by a distinct “ribbon” or “swirl” texture commonly found in ball clays.

Data from this study are not sufficient for complete petrogenetic interpretation. However, speculation on possible differences in depositional environments and modes of deposition can be based on the data at hand. The Blue Mountain variety is considered from previous studies to be primary. The Ashland variety is probably a first generation alluvial clay. The Sardis variety appears to be a multiple generation, detrital product that accumulated as part of overbank swamp deposits.

Low-temperature FTIR spectroscopy was used to characterize the v(OH) region of kaolin-group minerals including well ordered to poorly ordered kaolins from Georgia, Brazil, and England, along with samples of discrete dickite and nacrite. Low-temperature FTIR spectra were useful in resolving dickite- and nacrite-like features present in the spectra of kaolins when cooled to <30 K. These features were not resolved at room temperature and only partially resolved at liquid N2 temperature (77 K). The room-temperature and low-temperature positions of the ν(OH) bands of kaolinite, dickite, and nacrite were linearly correlated with the interatomic OH⋯O distances and this relationship served as the basis for polytype/disorder identification. Dickite or dickite-like disorder was found in high Hinckley-Index kaolinite from Keokuk, Iowa, and from Cornwall, England. Dickite- and nacrite-like features were observed in both high- and low-Hinckley-index kaolinite and the amounts of these stacking sequences generally increased with decreasing Hinckley Index.

The purpose of this report is to describe the appropriate use of indices relating to crystallinity, such as the ‘crystallinity index’, the ‘Hinckley index’, the ‘Kübler index’, and the ‘Árkai index’. A ‘crystalline’ solid is defined as a solid consisting of atoms, ions or molecules packed together in a periodic arrangement. A ‘crystallinity index’ is purported to be a measure of crystallinity, although there is uncertainty about what this means (see below). This report discusses briefly the nature of order, disorder and crystallinity in phyllosilicates and discusses why the use of a ‘crystallinity index’ should be avoided. If possible, it is suggested that indices be referred to using the name of the author who originally described the parameter, e.g. ‘Hinckley index’ or ‘Kübler index’, or in honor of a researcher who investigated the importance of the parameter extensively, e.g. ‘Árkai index’.

The purpose of this report is to describe the appropriate use of indices relating to crystallinity, such as the ‘crystallinity index’, the ‘Hinckley index’, the ‘Kü bler index’, and the ‘Árkai index’. A ‘crystalline’ solid is defined as a solid consisting of atoms, ions, or molecules packed together in a periodic arrangement. A ‘crystallinity index’ is purported to be a measure of crystallinity, although there is uncertainty about what this means (see below). This report discusses briefly the nature of order, disorder and crystallinity in phyllosilicates and discusses why the use of a ‘crystallinity index’ should be avoided. If possible, it is suggested that indices be referred to using the name of the author who originally described the parameter, as in ‘Hinckley index’ or ‘Kübler index’, or in honour of a researcher who investigated the importance of the parameter extensively, as in ‘Árkai index’.