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arXiv:1612.09410 · Nature Communications

Robust spin correlations at high magnetic fields in the harmonic honeycomb iridates

Kimberly A. Modic, Brad J. Ramshaw, Jonathan Betts, Nicholas Breznay, James G. Analytis, R. McDonald, Arkady Shekhter

Published Jul 26, 2017• 32 citations
arXivHTMLPDF

Abstract

The complex antiferromagnetic orders observed in the honeycomb iridates are a double-edged sword in the search for a quantum spin-liquid: both attesting that the magnetic interactions provide many of the necessary ingredients, while simultaneously impeding access. Focus has naturally been drawn to the unusual magnetic orders that hint at the underlying spin correlations. However, the study of any particular broken symmetry state generally provides little clue about the possibility of other nearby ground states. Here we use magnetic fields approaching 100 Tesla to reveal the extent of the spin correlations in γ-lithium iridate. We find that a small component of field along the magnetic easy-axis melts long-range order, revealing a bistable, strongly correlated spin state. Far from the usual destruction of antiferromagnetism via spin polarization, the high-field state possesses only a small fraction of the total iridium moment, without evidence for long-range order up to the highest attainable magnetic fields.The complex antiferromagnetic orders observed in the honeycomb iridates prevent access to a spin-liquid ground state. Here the authors apply extremely high magnetic fields to destroy the antiferromagnetic order in γ-lithium iridate and reveal a bistable, strongly correlated spin state.

DOI
10.1038/s41467-017-00264-6

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The complex antiferromagnetic orders observed in the honeycomb iridates are a double-edged sword in the search for a quantum spin-liquid: both attesting that the magnetic interactions provide many of the necessary ingredients, while simultaneously impeding access. Focus has naturally been drawn to the unusual magnetic orders that hint at the underlying spin correlations. However, the study of any particular broken symmetry state generally provides little clue about the possibility of other nearby ground states. Here we use magnetic fields approaching 100 Tesla to reveal the extent of the spin correlations in γ-lithium iridate. We find that a small component of field along the magnetic easy-axis melts long-range order, revealing a bistable, strongly correlated spin state. Far from the usual destruction of antiferromagnetism via spin polarization, the high-field state possesses only a small fraction of the total iridium moment, without evidence for long-range order up to the highest attainable magnetic fields.The complex antiferromagnetic orders observed in the honeycomb iridates prevent access to a spin-liquid ground state. Here the authors apply extremely high magnetic fields to destroy the antiferromagnetic order in γ-lithium iridate and reveal a bistable, strongly correlated spin state.
The magnetic-field response of the Mott-insulating honeycomb iridate Na2IrO3{\mathrm{Na}}_{2}{\mathrm{IrO}}_{3}Na2​IrO3​ is investigated using torque magnetometry measurements in magnetic fields up to 60 T. A peak-dip structure is observed in the torque response at magnetic fields corresponding to an energy scale close to the zigzag ordering ($\ensuremath{\approx}15\phantom{\rule{0.28em}{0ex}}\mathrm{K}$) temperature. Using exact diagonalization calculations, we show that such a distinctive signature in the torque response constrains the effective spin models for these classes of Kitaev materials to ones with dominant ferromagnetic Kitaev interactions, while alternative models with dominant antiferromagnetic Kitaev interactions are excluded. We further show that, at high magnetic fields, long range spin correlation functions decay rapidly, pointing to a transition to a long-sought-after field-induced quantum spin liquid beyond the peak-dip structure, suggesting this to be a common feature of the family of Kitaev systems. Kitaev systems are thus revealed to be excellent candidates for field-induced quantum spin liquids, similar physics having been suggested in another Kitaev system $\ensuremath{\alpha}\text{\ensuremath{-}}{\mathrm{RuCl}}_{3}$.
Due to the combination of a substantial spin-orbit coupling and correlation effects, iridium oxides hold a prominent place in the search for novel quantum states of matter, including, e.g., Kitaev spin liquids and topological Weyl states. We establish the promise of the very recently synthesized hyper-honeycomb iridate β-Li2IrO3 in this regard. A detailed theoretical analysis reveals the presence of large ferromagnetic first-neighbor Kitaev interactions, while a second-neighbor antiferromagnetic Heisenberg exchange drives the ground state from ferro to zigzag order via a three-dimensional Kitaev spin liquid and an incommensurate phase. Experiment puts the system in the latter regime but the Kitaev spin liquid is very close and reachable by a slight modification of the ratio between the second- and first-neighbor couplings, for instance via strain.
Due to the combination of a substantial spin-orbit coupling and correlation effects, iridium oxides hold a prominent place in the search for novel quantum states of matter, including, e.g., Kitaev spin liquids and topological Weyl states. We establish the promise of the very recently synthesized hyper-honeycomb iridate β-Li2IrO3 in this regard. A detailed theoretical analysis reveals the presence of large ferromagnetic first-neighbor Kitaev interactions, while a second-neighbor antiferromagnetic Heisenberg exchange drives the ground state from ferro to zigzag order via a three-dimensional Kitaev spin liquid and an incommensurate phase. Experiment puts the system in the latter regime but the Kitaev spin liquid is very close and reachable by a slight modification of the ratio between the second- and first-neighbor couplings, for instance via strain.
In this doctoral dissertation, we consider the significance of spin-orbit coupling for the phases of matter which arise for strongly correlated electrons. We explore emergent behavior in quantum many-body systems, including symmetry-breaking orders, quantum spin liquids, and unconventional superconductivity. Our study is cemented by a particular class of Mott-insulating materials, centered around a family of two- and three-dimensional iridium oxides, whose honeycomb-like lattice structure admits peculiar magnetic interactions, the so-called Kitaev exchange. By analyzing recent experiments on these compounds, we show that this unconventional exchange is the key ingredient in describing their magnetism, and then use a combination of numerical and analytical techniques to investigate the implications for the phase diagram as well as the physics of the proximate three-dimensional quantum spin liquid phases. These long-ranged-entangled fractionalized phases should exhibit special features, including finite-temperature stability as well as unconventional high-Tc superconductivity upon charge-doping, which should aid future experimental searches for spin liquid physics. Our study explores the nature of frustration and fractionalization which can arise in quantum systems in the presence of strong spin-orbit coupling.
We use tensor-network methods and high-order linked-cluster expansions to explore the quantum phase diagram of the antiferromagnetic Kitaev honeycomb model in a magnetic field for general spin S values. Tensor network calculations for the pure Kitaev model confirm the absence of fluxes and spin-spin correlations beyond nearest neighbors, while revealing discrete orientational symmetry breaking for S ∈ 1, 3/2, 2, consistent with the semiclassical limit. An intermediate region between Kitaev phases and the high-field polarized phase is identified for all considered spin values, showing a sequence of potential phases characterized by distinct local magnetization patterns while the total magnetization increases smoothly as a function of the field. Linked-cluster expansions for the high-field zero-momentum gap and spectral weight indicate a quantum critical breakdown of the polarized phase, suggesting exotic physics at intermediate Kitaev couplings. The antiferromagnetic spin 1/2 Kitaev model is known to have an intermediate phase under a magnetic field before transitioning to a fully polarized state. However, the nature of this phase for higher spins remained unclear. This paper explores the quantum phase diagram of the antiferromagnetic Kitaev honeycomb model in a magnetic field using tensor-network methods and high-order linked cluster expansions, uncovering an intermediate phase with distinct local magnetization patterns across different spin values.
The Kitaev quantum spin liquid has been among the most intensively studied states of matter but there has been no clear-cut materials realization of it. This absence is largely because all existing honeycomb lattices are inherently distorted and disordered, which inevitably amplifies the competing Heisenberg interaction in the Kitaev-Heisenberg model, leading to an unwanted antiferromagnetic state. This work reports a new, undistorted honeycomb iridate NaxIrO3{}_{3}3​, where all evidence indicates that the elusive Kitaev spin liquid may finally be within reach.