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Title: Quantum Versus Classical Spin Fragmentation in Dipolar Kagome Ice Ho 3 Mg 2 Sb 3 O 14

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 T*≈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 icelike components; and persistent inelastic magnetic excitations down to T≈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 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 themore » 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.« less

Authors:
ORCiD logo; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Georgia Institute of Technology, Atlanta, GA (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; National Science Foundation (NSF)
OSTI Identifier:
1668450
Alternate Identifier(s):
OSTI ID: 1673167; OSTI ID: 1798626
Grant/Contract Number:  
SC0018660; AC05-00OR22725; DMR-2003117
Resource Type:
Published Article
Journal Name:
Physical Review. X
Additional Journal Information:
Journal Name: Physical Review. X Journal Volume: 10 Journal Issue: 3; Journal ID: ISSN 2160-3308
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; Frustrated magnetism; Quantum spin liquid; Kagome lattice; Polycrystalline materials; Spin ice; Mean field theory; Neutron scattering; Random phase approximation; Semiclassical methods; Specific heat measurements; Time-of-flight neutron spectroscopy

Citation Formats

Dun, Zhiling, Bai, Xiaojian, Paddison, Joseph A. M., Hollingworth, Emily, Butch, Nicholas P., Cruz, Clarina D., Stone, Matthew B., Hong, Tao, Demmel, Franz, Mourigal, Martin, and Zhou, Haidong. Quantum Versus Classical Spin Fragmentation in Dipolar Kagome Ice Ho 3 Mg 2 Sb 3 O 14. United States: N. p., 2020. Web. doi:10.1103/PhysRevX.10.031069.
Dun, Zhiling, Bai, Xiaojian, Paddison, Joseph A. M., Hollingworth, Emily, Butch, Nicholas P., Cruz, Clarina D., Stone, Matthew B., Hong, Tao, Demmel, Franz, Mourigal, Martin, & Zhou, Haidong. Quantum Versus Classical Spin Fragmentation in Dipolar Kagome Ice Ho 3 Mg 2 Sb 3 O 14. United States. https://doi.org/10.1103/PhysRevX.10.031069
Dun, Zhiling, Bai, Xiaojian, Paddison, Joseph A. M., Hollingworth, Emily, Butch, Nicholas P., Cruz, Clarina D., Stone, Matthew B., Hong, Tao, Demmel, Franz, Mourigal, Martin, and Zhou, Haidong. Tue . "Quantum Versus Classical Spin Fragmentation in Dipolar Kagome Ice Ho 3 Mg 2 Sb 3 O 14". United States. https://doi.org/10.1103/PhysRevX.10.031069.
@article{osti_1668450,
title = {Quantum Versus Classical Spin Fragmentation in Dipolar Kagome Ice Ho 3 Mg 2 Sb 3 O 14},
author = {Dun, Zhiling and Bai, Xiaojian and Paddison, Joseph A. M. and Hollingworth, Emily and Butch, Nicholas P. and Cruz, Clarina D. and Stone, Matthew B. and Hong, Tao and Demmel, Franz and Mourigal, Martin and Zhou, Haidong},
abstractNote = {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 T*≈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 icelike components; and persistent inelastic magnetic excitations down to T≈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 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.},
doi = {10.1103/PhysRevX.10.031069},
journal = {Physical Review. X},
number = 3,
volume = 10,
place = {United States},
year = {2020},
month = {9}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1103/PhysRevX.10.031069

Figures / Tables:

FIG. 1 FIG. 1: Classical spin fragmentation (CSF) process in a model of dipolar kagome ice displaying emergent-charge order, based on Ref. [39]. The expectation values of spinsmore » $\langle$$σ^z_i$$\rangle$ are represented by black arrows. Each triangle has one spin pointing “in” (toward its center) and two pointing “out” (away from its center), or vice versa. The emergent magnetic charge of a triangle is defined as the number of spins pointing in minus the number pointing out. Positive ($Q_j$ = +) and negative ($Q_j$ = −) emergent charges are represented as red and blue triangles, respectively, and form a staggered arrangement. Three distinct spin configurations are possible for a given emergent charge, which yields a macroscopic number of degenerate spin configurations associated with emergent-charge ordering. Spin fragmentation decomposes each unit length spin into “divergence-full” and “divergence-free” channels (center and right-hand images, respectively). The fragmented spins are shown as orange circles with diameter proportional to the length of the fragmented spin. The green hexagon represents the flipping of six spins around a closed loop: this is the simplest process that connects two distinct spin configurations within the degenerate CSF manifold.« less

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