<p> The a-β phase transformation was studied in hydrothermally grown crystals of A1PO4 by measuring the spin-Hamiltonian parameters of Fe^3+ as a function of temperature. </p> <p> The theory of the Blume-Orbach mechanism for the zero-field splitting of s-state ions was generalized and used to calculate the D-tensor of the spin-Hamiltonian. The experimentally observed temperature variation of the spin-Hamiltonian was interpreted in terms of a temperature-dependent point-multipole model of the charge distribution in the crystal lattice. </p> <p> A similar study of the a-S phase transformation in quartz was attempted but E.P.R. measurements could only be taken up to 450°C (123°C below the transformation temperature) because of the instability of the Fe^3+ center at higher temperatures. </p> / Thesis / Doctor of Philosophy (PhD)