Quantum Versus Classical Spin Fragmentation in Dipolar Kagome Ice Ho3Mg2Sb3O14.

Abstract

A promising route to realize entangled magnetic states combines geometrical frustration with quantum-tunneling effects. Spin-ice materials are canonical examples of frustration, and Ising spins in a transverse magnetic field are the simplest many-body model of quantum tunneling. Here, we show that the tripod-kagome lattice material Ho3Mg2Sb3O14 unites an icelike magnetic degeneracy with quantum-tunneling terms generated by an intrinsic splitting of the Ho3+ ground-state doublet, which is further coupled to a nuclear spin bath. Using neutron scattering and thermodynamic experiments, we observe a symmetry-breaking transition at to a remarkable state with three peculiarities: a concurrent recovery of magnetic entropy associated with the strongly coupled electronic and nuclear degrees of freedom; a fragmentation of the spin into periodic and icelike components; and persistent inelastic magnetic excitations down to . These observations deviate from expectations of classical spin fragmentation on a kagome lattice, but can be understood within a model of dipolar kagome ice under a homogeneous transverse magnetic field, which we survey with exact diagonalization on small clusters and mean-field calculations. In Ho3Mg2Sb3O14, hyperfine interactions dramatically alter the single-ion and collective properties, and suppress possible quantum correlations, rendering the fragmentation with predominantly single-ion quantum fluctuations. Our results highlight the crucial role played by hyperfine interactions in frustrated quantum magnets and motivate further investigations of the role of quantum fluctuations on partially ordered magnetic states.