Polarized single crystal neutron diffraction study of the zero-magnetization ferromagnet ${\mathrm{Sm}}_{1-x}{\mathrm{Gd}}_x{\mathrm{Al}}_2 (x=0.024)$

We have determined the temperature evolution of the spin and orbital moments in the zero-magnetization ferromagnet ${\mathrm{Sm}}_{1-x}{\mathrm{Gd}}_x{\mathrm{Al}}_2$ ($x$ = 0.024) by combining polarized and unpolarized single crystal neutron diffraction data. The sensitivity of the polarized neutron technique has allowed the moment values to be determined with a precision of $\approx 0.1{\mu }_{\mathrm{B}}$. Our results clearly demonstrate that, when magnetized by a field of 8 T, the spin and orbital moments in ${\mathrm{Sm}}_{1-x}{\mathrm{Gd}}_x{\mathrm{Al}}_2$ are oppositely directed, so that the net magnetization is very small. Below 60 K the contributions from spin and orbital motions are both about $2{\mu }_{\mathrm{B}}$, with that due to orbital motion being slightly larger than that due to spin. Between 60 and 65 K the contributions of each to the magnetization fall rapidly and change sign at $T_{\mathrm{comp}} \approx 67\mathrm{K}$, above which the aligned moments recover but with the orbital magnetization still slightly higher than the spin one. These results imply that above $T_{\mathrm{comp}}$ the small resultant magnetization of the ${\mathrm{Sm}}^{3+}$ ion is oppositely directed to the magnetizing field. It is suggested that this anomaly is due to polarization of conduction electron spin associated with the doping ${\mathrm{Gd}}^{3+}$ ions.

Figure 1

Form factors [20] $\langle j_0\rangle$ and $\langle j_2\rangle$ for ${\mathrm{Sm}}^{3+}$.

Figure 2

The squares of the structure factors measured for crystal X1 at three temperatures plotted against their values calculated from model B. The inset shows the same plot for reflections measured from the smaller crystal, X2.

Figure 3

Variation with temperature of the spin and orbital contributions to the magnetization aligned by a field of 8 T in ${\mathrm{Sm}}_{0.976}{\mathrm{Gd}}_{0.024}{\mathrm{Al}}_2$.