The results of measurements at moderate to high magnetic fields on a large number of nonmagnetic ion substituted yttrium iron garnets suggest that intrasublattice interactions play an important role in determining their spontaneous magnetizations and Curie temperatures. It is shown that the system {Y3‐xCax} [Fe2] (Fe3‐xSix)O12 is continuously related to the system {Y3‐xCax}[ZrxFe2‐x](Fe3)O12 or {Y3} [ScxFe2‐x] (Fe3)O12. It is concluded that in these systems the tetrahedral‐tetrahedral (d‐d) antiferromagnetic interactions are stronger than octahedral‐octahedral (a‐a) antiferromagnetic interactions. The changes in magnetic structure from an ideal ferrimagnet, yttrium iron garnet, to an end‐member in which there are at least short‐range antiferromagnetic interactions (i.e., in {Ca3}[Fe2](Si3)O12 or a hypothetical {YCa2}[Zr2](Fe3)O12) should bear an analogy to the crystal chemical changes. It is therefore proposed that when substitution is made exclusively in one sublattice, the moments of the Fe3+ ions in that sublattice remain parallel (as in the Yafet‐Kittel theory), while the weakened average a‐d interactions and the intrasublattice interactions lead to random canting of the Fe3+ ion moments of the other. This tendency occurs as soon as substitution begins. On continued substitution, a point is reached beyond which canting increases much more rapidly with increasing substitution. In this region, the intrasublattice interactions dominate the a‐d interactions, but it is probable that the canting continues to be random.
In the {Y3}[MgxFe2‐x](Fe3‐xSix)O12 system, the point at which the tetrahedral intrasublattice interactions dominate is reached at about x = 0.95 as contrasted with x ≅ 0.70 for the {Y3‐xCax}[ZrxFe2‐x](Fe3)O12 and {Y3}[ScxFe2‐x](Fe3)O12 systems. The canting of the d‐site ion moments increases at the same rate in the three systems to x ≅ 0.70, but beyond this point, the canting in the Mg‐Si substituted YIG is always substantially less than for the other two systems. This together with data on other substituted garnets indicates that the substitution of the Si4+ ions in the d‐sites lends to decrease the average d‐d interaction strength. Similarly, substitution in the a sites tends to decrease the average a‐a interaction strength.
Measurements on some garnets in the systems {Y3‐yCay} [ScxFe2‐x]‐(SiyFe3‐y)O12, {Y3‐y+xCay‐x}[MgxFc2_x](Fe3‐vSiy)O12 and {Y3‐x‐yCax+y}‐[ZrxFe2‐x]{SiyFe3‐y)O12 indicate that different nonmagnetic ions may produce different magnetic behavior. This is especially noticeable in the region in which the intrasublattice interactions are dominant. Comparative behavior of the systems {Y3}[ScxFe2‐x](Fe3)O12 and {Y3‐xCax}[ZrxFe2‐x]‐(Fe3)O12 and of the systems {Y3‐xCax}[Fe2](Fe3‐xMx)O12, M ≡ Si and Ge, also indicates that the ion type is important in determining magnetic behavior. It is speculated that this results from effects on the interaction geometry, especially when the interactions are weak.
Results on garnets in systems {Y3‐yCay}[ScxFe2‐x](Fe3‐ySiy)O12, (Y3‐y+xCay‐x} [MgxFe2‐x](Fe3‐...