Quantum versus Classical Spin Fragmentation in Dipolar Kagome Ice Ho3Mg2Sb3O14

TL;DR

This paper investigates the interplay of quantum tunneling and spin fragmentation in the dipolar kagome ice material Ho3Mg2Sb3O14, revealing a unique symmetry-breaking transition with persistent excitations influenced by hyperfine interactions.

Contribution

It demonstrates how hyperfine interactions modify quantum and collective magnetic properties, leading to a novel state with spin fragmentation and persistent excitations in a kagome ice system.

Findings

Observation of a symmetry-breaking transition at 0.32 K

Detection of spin fragmentation into periodic and ice-like components

Persistent inelastic magnetic excitations down to 0.12 K

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 $T^{\ast}\approx0.32$ 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 $T\approx0.12$ 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.