Ice rule correlations in stuffed spin ice

Abstract

Stuffed spin ice is a chemical variation of a spin ice material like Ho _2 Ti _2 O _7 in which extra magnetic ions are inserted into the crystal structure. Previous studies have shown that the degree of stuffing has very little effect on the residual entropy in the system, which takes a value very close to the spin ice entropy. We argue, however, that the observation of this entropy does not imply long range coherence of the ice rules, that determine the local spin configurations. We have characterized deviations from the ice rules by means of a polarized neutron diffraction study of a single crystal of Ho _2+ _δ Ti _2− _δ O _7− _δ _/2 with δ = 0.3. Our results demonstrate that the ice rules in stuffed spin ice are strictly valid only over a relatively short range, and that at longer range stuffed spin ice exhibits some characteristics of a ‘cluster glass’, with a tendency to more conventional ferromagnetic correlations.