Influence of controlled disorder on the dipolar spin ice state of Ho-based pyrochlores

TL;DR

This study investigates how controlled chemical disorder affects the dipolar spin-ice state in Ho-based pyrochlores, revealing robustness of the state despite structural distortions and disorder-induced magnetic excitations.

Contribution

It demonstrates that the dipolar spin-ice state in Ho pyrochlores remains stable under various controlled disorder conditions, highlighting its robustness.

Findings

Both disordered compounds retain the dipolar spin-ice signatures.

Disorder induces broad magnetic excitations within the spin-ice regime.

Structural distortions and cation disorder are present but do not destroy the spin-ice state.

Abstract

Pyrochlore magnets of the form $R_2B_2$O$_7$, in which rare-earth ions on the $R$-site form a three-dimensional network of corner-sharing tetrahedra, provide a canonical setting for geometrical frustration. Ho-based pyrochlores host a dipolar spin-ice ground state, characterized by Ising moments constrained by the ice rules and elementary excitations analogous to magnetic monopoles. Here we examine how controlled chemical disorder influences this state by introducing site mixing on the non-magnetic $B$-site in two compounds. Ho$_2$GaSbO$_7$ contains only Ga$^{3+}$/Sb$^{5+}$ charge disorder, whereas Ho$_2$ScSbO$_7$ exhibits both charge and substantial size disorder arising from the large ionic-radius mismatch between Sc$^{3+}$ and Sb$^{5+}$. Although both materials retain the pyrochlore structure, neutron scattering measurements reveal a reduced correlation length for the $R/B$-site cation ordering and enhanced local structural distortions in Ho$_2$ScSbO$_7$. Despite these structural differences, bulk thermodynamic measurements and magnetic diffuse scattering demonstrate that both systems exhibit the defining signatures of a dipolar spin-ice state. Low-energy inelastic neutron spectroscopy further uncovers broad magnetic excitations that develop within the dipolar spin-ice regime, a feature absent in pristine Ho pyrochlores and indicative of disorder-induced splitting of the non-Kramers ground-state doublet. Together, these results show that controlled disorder generates tunable transverse-field-driven quantum fluctuations in Ho-based pyrochlores, although the dipolar spin-ice state is remarkably robust to this disorder.