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

Adam A. Aczel1,*, Brenden R. Ortiz2, Yi Luo1, Ganesh Pokharel3,†, Paul M. Sarte3, Clarina dela Cruz1, Jue Liu1, Gabriele Sala4,‡, Stephen D. Wilson5 et al.

Benjamin A. Frandsen6 and Joseph A. M. Paddison1

  • *Contact author: aczelaa@ornl.gov
  • †Present address: Perry College of Mathematics, Computing, and Sciences, University of West Georgia, Carrollton, Georgia 30118, USA.
  • ‡Present address: Materials and Life Science Division, J-PARC Center, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195, Japan.

Phys. Rev. B 113, 214415 – Published 3 June, 2026

DOI: https://doi.org/10.1103/pvl4-vxzx

Abstract

Pyrochlore magnets of the form R2B2O7, 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 nonmagnetic B site in two compounds. Ho2GaSbO7 contains only Ga3+/Sb5+ charge disorder, whereas Ho2ScSbO7 exhibits both charge and substantial size disorder arising from the large ionic-radius mismatch between Sc3+ and Sb5+. 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 Ho2ScSbO7. 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.

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