Chemical and optical data are presented for the orthopyroxenes, clinopyroxenes, garnets, plagioclases, and opaque oxides in high-grade regionally metamorphosed basic rocks and their garnetiferous associates from the Willyama Complex. Exsolution phenomena in the pyroxenes have been studied by X-ray diffraction methods and with the electron probe micro-analyser. The (001) lamellae in one lime-rich clinopyroxene are clinohypersthene. Comparison of the Willyama and other granulite facies clinopyroxenes with those of slowly cooled basic igneous rocks suggests that their chemical compositions may be used as guides to temperature conditions during formation. Willyama plagioclases are complexly twinned and possess intermediate structural states.

A full-matrix, three-dimensional refinement of kalsilite, KAlSi04 (hexagonal, a 5·16, c 8.69 Å, P6a), shows that the silicon and aluminium atoms are ordered. The respective tetrahedral distances of 1·61 and 1·74 Å agree with values of 1·61 and 1·75 Å taken to be typical of framework structures. As in nepheline, an oxygen atom is statistically distributed over three sites displaced 0·25 Å from the ideal position on a triad axis. This decreases the bond angle from 180° to 163° in conformity with observations on some other crystal structures. The potassiumoxygen distances of 2·77, 2·93, and 2·99 Å are consistent with the wide range normally found for this weakly bonded atom.

Leucite and pseudoleucite invariably have lower K/Rb ratios and higher K/Sr and K/Ba ratios than the groundmasses of the rocks in which they occur. The distribution of Rb, Sr, and Ba between K-rich minerals (e.g. alkali feldspars) and the liquids from which they crystallize is generally such that Rb is impoverished and Sr and Ba enriched, relative to K, in the crystallizing phase. Leucite shows the opposite relationship and this is attributed to the leucite structure being sensitive to the size and valency of the ions replacing K.

The electron probe was used to analyse for Fe, Ti, Mg, Al, and Mn. Vanadium could not be determined because of interference from Ti. Calcium was shown to be present only in inclusions of apatite and silicate; it does not oceur in the titanomagnetite structure.

Homogeneous grains (magnetite-ulvöspinel solid solutions) do not vary greatly in bulk composition, averaging close to 61% Fe and 8 % TiO2. Inhomogeneous grains contain variable amounts of hematite-ilmenite lamellae produced by progressive oxidation of the homogeneous grains. In the early stages there is rapid build-up of titanium in the rhombohedral lamellae, which are initially relatively poor in iron. As oxidation proceeds the almost titanium-free cubic phase becomes strongly enriched in magnesium, aluminium, and manganese, while the iron: titanium ratio in the rhombohedral phase increases. The end-product may be a homogeneous titanhematite, if initial concentrations of Mg, Al, and Mn are low. Otherwise residuals of a relatively iron-poor almost titanium-free (Mg, Al, Mn)-enriched cubic phase remain in the titanhematite. The behaviour of iron and titanium agrees with recent synthetic work in the system. Some of the oxidized grains contain transparent spinel lamellae exsolved from the cubic phase. Exsolution may commence at different stages in the oxidation process, but the reason is not clear—there are no significant differences in the composition of phases with and without spinel lamellae.

Analyses and normative compositions are presented for the different phases in each grain, where possible. The compositional changes accompanying oxidation satisfactorily explain the slope of the thermomagnetic curves : there is no need to invoke bulk compositional variations within a given ironsand sample.

Samples from an ilmenite and a non-titaniferous magnetite concentrate were also briefly examined.

A new occurrence of varlamoffite is described, and the status of this species is considered; the term is best employed for cryptocrystalline yellowish material consisting predominantly of Sn and H20 that may yield a diffuse powder pattern comparable to, or closely resembling that of cassiterite, but does yield a powder pattern identical with that of cassiterite after heat-treatment at about 1200° C. A new mineral, malayaite, CaSnSiO5, is briefly described; it is isostructural with sphene.

In the Donegal Granite garnet occurs as an accessory mineral in muscovite-granties, pegmatites, and aplites. The composition of the garnet in fourteen samples of granitic rock has been determined from the physical properties and three new chemical analyses are given. All the samples examined are intermediate in composition between almandine and spessartine. The reason for the high manganese content in garnet from granites is discussed.

The transformation of ankerite during heat treatment has been studied by single-crystal and powder X-ray methods. The mechanisms of formation of calcite at 750° C and of periclase at 950° C are discussed from a structural viewpoint.

Tables are given which enable a quick estimate to be made of the true thickness of kamacite plates from measurements of the Widmanstetter figure on a single random plane. The method is applied to the following meteorites (width in mm following name): Arispe, 2·90; Brenham, 0·91; Duketon, 1·13; Henbury, 0·74; Ogallala, 1·53; Thule, 0·89; View Hill, 0·62.

Psilomelane has been redefined from single crystal study to be of orthorhombic symmetry with the space group P222, the dimensions a 9·45, b 13·90, c 5·72 Å, and two molecules of per unit cell, where A represents Ba2+, Mn2+, Al3+, Fe3+, Si4+ etc., and X6 stands for (O,OH)6 with OH about 5. This formula is very closely followed by 14 analyses of psilomelane, and the calculated density agrees fairly well with the observed density. The powder data of psilomelane cannot be indexed with Wadsley's monoclinic cell and the conditions for the space group A2/m, proposed by Wadsley for his crystal, are not satisfied by the indexing. Wadsley's crystal was not psilomelane but probably an altered phase of Vaux's neotype specimen.

The electron micrograph of shining platy crystals of psilomelane shows some almost square-faced crystals whereas that of the botryoidal material consists only of particles with irregular edges. The dehydration product of psilomelane shows gradual shrinkage of the orthorhombic cell up to 500° C, marked structural changes at 600° C, and transformation at 800° C to a monoclinic phase, similar to hollandite.

The Equivibration Curve technique of Joel (1963) is used to determine the orientation of a zoned mineral on the spindle stage axis and an average value for 2V. A bracketing method enables the extreme values of each refractive index to be determined for sodium light on a single grain, using the Focal-plane Screening technique of Cherkosov (1960).