A magnetic, neutron-diffraction, and Mössbauer spectral study of the Ce2Fe17−xSix solid solutions

Abstract

The magnetic properties of a series of Ce2Fe17−xSix solid solutions with x equal to 0.0, 0.23, 0.4, 0.6, 0.8, 1.02, 1.98, and 3.20 have been studied by magnetic measurements, neutron diffraction, and Mössbauer spectroscopy. An x-ray-diffraction study indicates that the compounds adopt the rhombohedral Th2Zn17-type structure. The substitution of silicon for iron in Ce2Fe17 leads to a contraction of the a axis by 0.2%, an expansion of the c axis by 0.2%, and a consequent reduction of the unit-cell volume by about 0.2% per substituted silicon. Magnetization studies indicate that the Curie temperature increases uniformly from 238 K for Ce2Fe17 to 455 K for Ce2Fe14Si2. Powder neutron-diffraction results, obtained at 295 K, indicate both that the silicon atoms preferentially occupy the 18h sites and that the iron moments increase with increasing silicon content, an increase which is related to the increase in Curie temperature. The Mössbauer spectra have been fit with a binomial distribution of the near-neighbor environments in terms of a maximum hyperfine field Hmax for an iron with zero silicon near neighbors, and a decremental field ΔH per silicon near neighbor. The compositional independence of both the weighted average maximum hyperfine field and of the decremental field indicates that the silicon acts as a magnetic hole, a hole which does not perturb the magnetic moments at the iron sites. The compositional dependence of the weighted average isomer shift is explained in terms of an interband mixing of the iron 4s and silicon 2p bands, due to the reduction of the iron 18h bond lengths. This interband mixing affects the charge but not the spin distribution at the iron sites.