TEM and XRD determination of crystallite size and lattice strain as a function of illite crystallinity in pelitic rocks

Average crystallite size and mean-square strain of illite in rock specimens and clay separates were measured independently in TEM images and by single-line Fourier (Voigt method) profile analysis of the c. 1 nm peak of XRD patterns for a prograde sequence of pelitic rocks (illite crystallinity indices = 0.17-0.58° Δ2θ) from the Gaspé Peninsula, Quebec. The TEM-determined crystallite sizes in clay separates approximate those determined by Fourier profile analyses and those calculated from illite crystallinity indices by the Scherrer equation, with the exception of the diagenetic sample. The crystallite sizes and mean-square strains of illite in rock samples exhibit a trend similar to that determined by profile analyses, but the average crystallite sizes are up to five times larger than those measured for clay separates. TEM images show that all rock samples have a wide range of crystallite sizes, and the proportions of larger crystallites increase with metamorphic grade. The diagenetic illite is defect-rich, fine-grained (mean thickness by volume=c. 70 nm), 1M_d material. Anchizonal illite tends to occur as separate aggregates of small 1M_d and larger 2M₁ crystals (c. 200 nm), comprising arrays of subparallel coalescing packets. The epizone sample has thick (c. 400 nm), defect-free crystals of muscovite occurring in stacks of parallel layers, or subhedral crystals intergrown with large-angle boundaries. Cleaved crystals that are free of intracrystalline layer terminations are dominant in clay separates of all samples, having ranges of smaller sizes with volume-average thicknesses of c. 43, 43, and 81 nm (c. 14, 28, 67 nm by the Voigt method), respectively, for the three zones. The results suggest that illite crystallinity indices do not provide a direct measure of a single microstructural state of illite in rocks, although they yield consistent limits for average crystallite sizes for the anchizone (23 & 48 nm here). Therefore, they serve as a general parameter of the degree of recrystallization on a relative basis, in part because the contributions of all peak-broadening variables (mixed layering, size and strain) decrease regularly with prograde regional metamorphism of pelites. The microstructural changes caused by rock disaggregation are probably a function of those variables as well. The data collectively demonstrate a trend from metastable, defect-rich, small crystals towards a stable assemblage of larger, defect-free crystals, through dissolution of strained crystals and neocrystallization, consistent with the Ostwald step rule.