DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Momentum-independent magnetic excitation continuum in the honeycomb iridate H3LiIr2O6

Journal Article · · Nature Communications
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2];  [3];  [3]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [4]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [1]
  1. Brown Univ., Providence, RI (United States)
  2. Boston College, Chestnut Hill, MA (United States)
  3. Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
  4. Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)

Understanding the interplay between the inherent disorder and the correlated fluctuating-spin ground state is a key element in the search for quantum spin liquids. H3LiIr2O6 is considered to be a spin liquid that is proximate to the Kitaev-limit quantum spin liquid. Its ground state shows no magnetic order or spin freezing as expected for the spin liquid state. However, hydrogen zero-point motion and stacking faults are known to be present. The resulting bond disorder has been invoked to explain the existence of unexpected low-energy spin excitations, although data interpretation remains challenging. Here, we use resonant X-ray spectroscopies to map the collective excitations in H3LiIr2O6 and characterize its magnetic state. In the low-temperature correlated state, we reveal a broad bandwidth of magnetic excitations. The central energy and the high-energy tail of the continuum are consistent with expectations for dominant ferromagnetic Kitaev interactions between dynamically fluctuating spins. Furthermore, the absence of a momentum dependence to these excitations are consistent with disorder-induced broken translational invariance. Our low-energy data and the energy and width of the crystal field excitations support an interpretation of H3LiIr2O6 as a disordered topological spin liquid in close proximity to bond-disordered versions of the Kitaev quantum spin liquid.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States); Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Brown Univ., Providence, RI (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
Sponsoring Organization:
National Science Foundation (NSF); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-05CH11231; AC02-06CH11357; SC0021265
OSTI ID:
1995855
Journal Information:
Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 14; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

References (54)

Possible quantum paraelectric state in Kitaev spin liquid candidate H3LiIr2O6 journal August 2020
Anyons in an exactly solved model and beyond journal January 2006
Disorder upon disorder: Localization effects in the Kitaev spin liquid journal May 2021
A spin–orbital-entangled quantum liquid on a honeycomb lattice journal February 2018
Proximate Kitaev quantum spin liquid behaviour in a honeycomb magnet journal April 2016
Fractional spinon excitations in the quantum Heisenberg antiferromagnetic chain journal June 2013
Direct evidence for dominant bond-directional interactions in a honeycomb lattice iridate Na2IrO3 journal May 2015
Fermionic response from fractionalization in an insulating two-dimensional magnet journal July 2016
Scaling and data collapse from local moments in frustrated disordered quantum spin systems journal October 2018
Continuum of quantum fluctuations in a three-dimensional S = 1 Heisenberg magnet journal October 2018
Concept and realization of Kitaev quantum spin liquids journal March 2019
Single crystal growth from separated educts and its application to lithium transition-metal oxides journal October 2016
Solution of the heavily stacking faulted crystal structure of the honeycomb iridate H 3 LiIr 2 O 6 journal January 2017
Structure, and magnetic and electrochemical properties of layered oxides, Li2IrO3 journal February 2003
Quantum spin liquids: a review journal November 2016
Probing the continuum scattering and magnetic collapse in single-crystalline α − L i 2 Ir O 3 by Raman spectroscopy journal May 2020
Quantum paraelectricity in the Kitaev quantum spin liquid candidates H 3 LiI r 2 O 6 and D 3 LiI r 2 O 6 journal May 2020
Magnetic Raman continuum in single-crystalline H 3 LiIr 2 O 6 journal May 2020
Thermodynamic and transport properties in disordered Kitaev models journal August 2020
Optical magnons with dominant bond-directional exchange interactions in the honeycomb lattice iridate α − Li 2 IrO 3 journal January 2021
Enhanced hybridization in the electronic ground state of the intercalated honeycomb iridate Ag 3 Li Ir 2 O 6 journal September 2021
Coexistence of random singlets and disordered Kitaev spin liquid in H3LiIr2O6 journal January 2023
Antiferromagnetic Mott insulating state in single crystals of the honeycomb lattice material Na 2 IrO 3 journal August 2010
Mixing between J eff = 1 2 and 3 2 orbitals in Na 2 IrO 3 : A spectroscopic and density functional calculation study journal August 2013
α − RuCl 3 : A spin-orbit assisted Mott insulator on a honeycomb lattice journal July 2014
Thermal fractionalization of quantum spins in a Kitaev model: Temperature-linear specific heat and coherent transport of Majorana fermions journal September 2015
Dynamics of fractionalization in quantum spin liquids journal September 2015
Static and dynamical spin correlations of the S = 1 2 random-bond antiferromagnetic Heisenberg model on the triangular and kagome lattices journal October 2015
Clues and criteria for designing a Kitaev spin liquid revealed by thermal and spin excitations of the honeycomb iridate Na 2 IrO 3 journal May 2016
Extracting paramagnon excitations from resonant inelastic x-ray scattering experiments journal June 2016
Correlated impurities and intrinsic spin-liquid physics in the kagome material herbertsmithite journal August 2016
Relation between Kitaev magnetism and structure in α − RuCl 3 journal May 2017
Resonant inelastic x-ray scattering operators for t 2 g orbital systems journal August 2017
Theory of a quantum spin liquid in the hydrogen-intercalated honeycomb iridate H 3 LiIr 2 O 6 journal March 2018
Dynamics of a quantum spin liquid beyond integrability: The Kitaev-Heisenberg- Γ model in an augmented parton mean-field theory journal April 2018
Mott Insulators in the Strong Spin-Orbit Coupling Limit: From Heisenberg to a Quantum Compass and Kitaev Models journal January 2009
Relevance of the Heisenberg-Kitaev Model for the Honeycomb Lattice Iridates A 2 IrO 3 journal March 2012
Crystal-Field Splitting and Correlation Effect on the Electronic Structure of A 2 IrO 3 journal February 2013
Generic Spin Model for the Honeycomb Iridates beyond the Kitaev Limit journal February 2014
Dynamics of a Two-Dimensional Quantum Spin Liquid: Signatures of Emergent Majorana Fermions and Fluxes journal May 2014
Scattering Continuum and Possible Fractionalized Excitations in α − RuCl 3 journal April 2015
Resonant Inelastic X-Ray Scattering Response of the Kitaev Honeycomb Model journal September 2016
Disorder-Induced Mimicry of a Spin Liquid in YbMgGaO 4 journal October 2017
Strong Effect of Hydrogen Order on Magnetic Kitaev Interactions in H 3 LiIr 2 O 6 journal November 2018
Role of Hydrogen in the Spin-Orbital-Entangled Quantum Liquid Candidate H 3 LiIr 2 O 6 journal December 2018
Bond-Disordered Spin Liquid and the Honeycomb Iridate H 3 LiIr 2 O 6 : Abundant Low-Energy Density of States from Random Majorana Hopping journal February 2019
Disorder, Low-Energy Excitations, and Topology in the Kitaev Spin Liquid journal July 2022
Scaling Studies of Highly Disordered Spin-½ Antiferromagnetic Systems journal February 1982
Electronic ground state of two nonmagnetic pentavalent honeycomb iridates journal August 2022
Fingerprints of Kitaev physics in the magnetic excitations of honeycomb iridates journal October 2020
Disorder effects in the Kitaev-Heisenberg model journal April 2023
Quantum spin liquids journal January 2020
Spin-Orbit Physics Giving Rise to Novel Phases in Correlated Systems: Iridates and Related Materials journal March 2016
Metastable Kitaev Magnets journal January 2022