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 Ho${}_3$Mg${}_2$Sb${}_3$O${}_{14}$ unites an ice-like magnetic degeneracy with quantum-tunneling terms generated by an intrinsic splitting of the Ho${}^{3+}$ 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 $T^{\ast }\approx 0.32$ K 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 ice-like components; and persistent inelastic magnetic excitations down to $T\approx 0.12$ K. 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 Ho${}_3$Mg${}_2$Sb${}_3$O${}_{14}$, 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.

arXiv commentThe present manuscript elaborates on an earlier preprint, arXiv:1806.04081, from which it is significantly different

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