In 1967, Holtzberg, Gambino, and McGuire [J. Phys. Chem. Solids 28, 2283 (1967)] observed that intermetallic Gd5Si4 exhibits TC = 336 K. This is remarkable in that the TC of Gd (∼291 K) is increased by chemical union with a nontransition metal, which is rare, if not unique. In the present study, magnetization‐temperature behavior of Gd5Si4 and (Gd1−xMx)5Si4 systems with M=La or Y were studied and compared with the Brillouin function (BF) to see if molecular‐field theory is obeyed. Demagnetization near TC is much sharper for the alloys than expected from the BF. As examples, at T/TC = 0.9, the BF for Gd5Si4 gives M/M0 = 0.38, whereas the observed values range from 0.99 [for (Gd0.8Y0.2)5Si4] to 0.5 [for (Gd0.6La0.4)5Si4]. The factors responsible for these strong deviations from the BF and the high‐TC values of these alloys are as yet unclear. X‐ray patterns for yttrium‐doped samples with x=0.1–0.5 and La with x=0.05 and 0.1 appear identical to the pattern for Gd5Si4, indicating no structural change. For La substitution of x=0.2 and above, there is a change from orthorhombic to tetragonal structure. All of the compounds show a decrease in Curie temperature and magnetic moment as Gd is decreased, as expected because of the replacement of Gd by a nonmagnetic species.

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