Realization of a three-dimensional spin–anisotropic harmonic honeycomb iridate

Modic, K. A.; Smidt, Tess E.; Kimchi, Itamar; Breznay, Nicholas P.; Biffin, Alun; Choi, Sungkyun; Johnson, Roger D.; Coldea, Radu; Watkins-Curry, Pilanda; McCandless, Gregory T.; Chan, Julia Y.; Gandara, Felipe; Islam, Z.; Vishwanath, Ashvin; Shekhter, Arkady; McDonald, Ross D.; Analytis, James G.

doi:10.1038/ncomms5203

Title: Realization of a three-dimensional spin–anisotropic harmonic honeycomb iridate

Abstract

Spin and orbital quantum numbers play a key role in the physics of Mott insulators, but in most systems they are connected only indirectly—via the Pauli exclusion principle and the Coulomb interaction. Iridium-based oxides (iridates) introduce strong spin–orbit coupling directly, such that these numbers become entwined together and the Mott physics attains a strong orbital character. In the layered honeycomb iridates this is thought to generate highly spin–anisotropic magnetic interactions, coupling the spin to a given spatial direction of exchange and leading to strongly frustrated magnetism. Here we report a new iridate structure that has the same local connectivity as the layered honeycomb and exhibits striking evidence for highly spin–anisotropic exchange. The basic structural units of this material suggest that a new family of three-dimensional structures could exist, the ‘harmonic honeycomb’ iridates, of which the present compound is the first example.

Authors:

Modic, K. A. ^[1]; Smidt, Tess E. ^[2]; Kimchi, Itamar ^[3]; Breznay, Nicholas P. ^[2]; Biffin, Alun ^[4]; Choi, Sungkyun ^[4]; Johnson, Roger D. ^[4]; Coldea, Radu ^[4]; Watkins-Curry, Pilanda ^[5]; McCandless, Gregory T. ^[5]; Chan, Julia Y. ^[5]; Gandara, Felipe ^[6]; Islam, Z. ^[7]; Vishwanath, Ashvin ^[2]; Shekhter, Arkady ^[8]; McDonald, Ross D. ^[8]; Analytis, James G. ^[2]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. of Texas, Austin, TX (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States)
Univ. of Oxford (United Kingdom). Clarendon Lab.
Univ. of Texas at Dallas, Richardson, TX (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Publication Date:: Fri Jun 27 00:00:00 EDT 2014

Research Org.:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; National Science Foundation (NSF); Engineering and Physical Sciences Research Council (EPSRC), United Kingdom

OSTI Identifier:: 1581219

Grant/Contract Number:: AC02-05CH11231; DGE 1106400; EP/H014934/1

Resource Type:: Accepted Manuscript

Journal Name:: Nature Communications

Additional Journal Information:: Journal Volume: 5; Journal Issue: 1; Journal ID: ISSN 2041-1723

Publisher:: Nature Publishing Group

Country of Publication:: United States

Language:: English

Subject:: 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS

Citation Formats


                    Modic, K. A., Smidt, Tess E., Kimchi, Itamar, Breznay, Nicholas P., Biffin, Alun, Choi, Sungkyun, Johnson, Roger D., Coldea, Radu, Watkins-Curry, Pilanda, McCandless, Gregory T., Chan, Julia Y., Gandara, Felipe, Islam, Z., Vishwanath, Ashvin, Shekhter, Arkady, McDonald, Ross D., and Analytis, James G. Realization of a three-dimensional spin–anisotropic harmonic honeycomb iridate.  United States: N. p., 2014. 
Web.  doi:10.1038/ncomms5203.

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                    Modic, K. A., Smidt, Tess E., Kimchi, Itamar, Breznay, Nicholas P., Biffin, Alun, Choi, Sungkyun, Johnson, Roger D., Coldea, Radu, Watkins-Curry, Pilanda, McCandless, Gregory T., Chan, Julia Y., Gandara, Felipe, Islam, Z., Vishwanath, Ashvin, Shekhter, Arkady, McDonald, Ross D., & Analytis, James G. Realization of a three-dimensional spin–anisotropic harmonic honeycomb iridate.  United States.  https://doi.org/10.1038/ncomms5203

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                    Modic, K. A., Smidt, Tess E., Kimchi, Itamar, Breznay, Nicholas P., Biffin, Alun, Choi, Sungkyun, Johnson, Roger D., Coldea, Radu, Watkins-Curry, Pilanda, McCandless, Gregory T., Chan, Julia Y., Gandara, Felipe, Islam, Z., Vishwanath, Ashvin, Shekhter, Arkady, McDonald, Ross D., and Analytis, James G. Fri .  
"Realization of a three-dimensional spin–anisotropic harmonic honeycomb iridate".  United States.  https://doi.org/10.1038/ncomms5203.  https://www.osti.gov/servlets/purl/1581219.

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@article{osti_1581219,

  title        = {Realization of a three-dimensional spin–anisotropic harmonic honeycomb iridate},

  author       = {Modic, K. A. and Smidt, Tess E. and Kimchi, Itamar and Breznay, Nicholas P. and Biffin, Alun and Choi, Sungkyun and Johnson, Roger D. and Coldea, Radu and Watkins-Curry, Pilanda and McCandless, Gregory T. and Chan, Julia Y. and Gandara, Felipe and Islam, Z. and Vishwanath, Ashvin and Shekhter, Arkady and McDonald, Ross D. and Analytis, James G.},

  abstractNote = {Spin and orbital quantum numbers play a key role in the physics of Mott insulators, but in most systems they are connected only indirectly—via the Pauli exclusion principle and the Coulomb interaction. Iridium-based oxides (iridates) introduce strong spin–orbit coupling directly, such that these numbers become entwined together and the Mott physics attains a strong orbital character. In the layered honeycomb iridates this is thought to generate highly spin–anisotropic magnetic interactions, coupling the spin to a given spatial direction of exchange and leading to strongly frustrated magnetism. Here we report a new iridate structure that has the same local connectivity as the layered honeycomb and exhibits striking evidence for highly spin–anisotropic exchange. The basic structural units of this material suggest that a new family of three-dimensional structures could exist, the ‘harmonic honeycomb’ iridates, of which the present compound is the first example.},

  doi          = {10.1038/ncomms5203},

  journal      = {Nature Communications},

  number       = 1,

  volume       = 5,

  place        = {United States},

  year         = {Fri Jun 27 00:00:00 EDT 2014},

  month        = {Fri Jun 27 00:00:00 EDT 2014}

}

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DOI: 10.48550/arxiv.1707.03140

Topological semimetals and insulators in three-dimensional honeycomb materials
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Wawrzik, Dennis; Lindner, David; Hermanns, Maria
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DOI: 10.48550/arxiv.1803.04976

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Kunst, Flore K.; van Miert, Guido; Bergholtz, Emil J.
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Yamada, Masahiko G.
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Chakraborty, Jayita; Ganguli, Nirmal
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DOI: 10.48550/arxiv.2012.11868

Kitaev magnetism through the prism of lithium iridate
text, January 2021

Tsirlin, Alexander A.; Gegenwart, Philipp
arXiv
DOI: 10.48550/arxiv.2103.14073

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Title: Realization of a three-dimensional spin–anisotropic harmonic honeycomb iridate

Abstract

Citation Formats

Exactly solvable Kitaev model in three dimensions journal, January 2009

Competitions in Layered Ruthenates: Ferromagnetism versus Antiferromagnetism and Triplet versus Singlet Pairing journal, May 1999

NaIrO3—A pentavalent post-perovskite journal, March 2011

Simple Models of Magnetism book, January 2008

Zigzag Magnetic Order in the Iridium Oxide Na 2 IrO 3 journal, February 2013

Anyons in an exactly solved model and beyond journal, January 2006

Mott Insulators in the Strong Spin-Orbit Coupling Limit: From Heisenberg to a Quantum Compass and Kitaev Models journal, January 2009

Cuprate Superconductivity: Dependence of T c on the c -Axis Layering Structure journal, July 1999

Absence of Ferromagnetism or Antiferromagnetism in One- or Two-Dimensional Isotropic Heisenberg Models journal, November 1966

Torque magnetometry in pulsed magnetic fields with use of a commercial microcantilever journal, August 2002

Physical properties of the n =3 Ruddlesden - Popper compound journal, November 1998

Kitaev-Heisenberg Model on a Honeycomb Lattice: Possible Exotic Phases in Iridium Oxides A 2 IrO 3 journal, July 2010

Three-dimensional quantum spin liquids in models of harmonic-honeycomb iridates and phase diagram in an infinite- D approximation journal, November 2014

Heisenberg-Kitaev model on the hyperhoneycomb lattice journal, January 2014

Hybrid Improper Ferroelectricity: A Mechanism for Controllable Polarization-Magnetization Coupling journal, March 2011

Structure and properties of ordered Li2IrO3 and Li2PtO3 journal, August 2008

Magnetic Field-Tuned Quantum Criticality in the Metallic Ruthenate Sr3Ru2O7 journal, October 2001

Experimentally determining the exchange parameters of quasi-two-dimensional Heisenberg magnets journal, August 2008

Relevance of the Heisenberg-Kitaev Model for the Honeycomb Lattice Iridates A 2 IrO 3 journal, March 2012

Spin Waves and Revised Crystal Structure of Honeycomb Iridate Na 2 IrO 3 journal, March 2012

Magnetic excitation spectrum of Na 2 IrO 3 probed with resonant inelastic x-ray scattering journal, June 2013

Exactly solvable Kitaev model in three dimensions text, January 2008

Heisenberg-Kitaev model on hyperhoneycomb lattice text, January 2013

Three dimensional quantum spin liquids in models of harmonic-honeycomb iridates and phase diagram in an infinite-D approximation text, January 2013

Anyons in an exactly solved model and beyond text, January 2005

Ab Initio Approaches for Low‐Energy Spin Hamiltonians journal, March 2019

Comparative study of monolithic platinum and iridium as oxygen-evolving anodes during the electrolytic reduction of uranium oxide in a molten LiCl–Li2O electrolyte journal, February 2019

Iridates from the molecular side journal, July 2016

Raman spectroscopic signature of fractionalized excitations in the harmonic-honeycomb iridates β- and γ-Li2IrO3 journal, July 2016

Proximate Kitaev quantum spin liquid behaviour in a honeycomb magnet journal, April 2016

Evidence for anionic redox activity in a tridimensional-ordered Li-rich positive electrode β-Li2IrO3 journal, February 2017

Direct evidence for dominant bond-directional interactions in a honeycomb lattice iridate Na2IrO3 journal, May 2015

Correlated states in β-Li2IrO3 driven by applied magnetic fields journal, October 2017

Theory of the field-revealed Kitaev spin liquid journal, June 2019

Path to stable quantum spin liquids in spin-orbit coupled correlated materials journal, April 2018

Concept and realization of Kitaev quantum spin liquids journal, March 2019

Kitaev exchange and field-induced quantum spin-liquid states in honeycomb α-RuCl3 journal, November 2016

The 2016 oxide electronic materials and oxide interfaces roadmap journal, October 2016

Recent progress on correlated electron systems with strong spin–orbit coupling journal, August 2016

Quantum spin liquids: a review journal, November 2016

Barrier tunneling of the loop-nodal semimetal in the hyperhoneycomb lattice journal, April 2018

Resonant inelastic x-ray scattering study of $\alpha$ -RuCl 3 : a progress report journal, January 2020

The challenge of spin–orbit-tuned ground states in iridates: a key issues review journal, February 2018

Frustration and quantum criticality journal, May 2018

Residual entropy and spin fractionalizations in the mixed-spin Kitaev model journal, September 2019

All-oxide ferromagnetic resonance and spin pumping with SrIr O 3 journal, September 2019

Lattice dynamics and structural transition of the hyperhoneycomb iridate β − Li 2 IrO 3 investigated by high-pressure Raman scattering journal, February 2020

Spin dynamics and field-induced magnetic phase transition in the honeycomb Kitaev magnet α − Li 2 IrO 3 journal, February 2019

Universal tensor-network algorithm for any infinite lattice journal, May 2019

Non-Kitaev spin liquids in Kitaev materials journal, May 2019

Antiferromagnetic Kitaev interaction in f -electron based honeycomb magnets journal, June 2019

Hidden Plaquette Order in a Classical Spin Liquid Stabilized by Strong Off-Diagonal Exchange journal, June 2019

Crystal growth and magnetic anisotropy in the spin-chain ruthenate Na 2 RuO 4 journal, February 2018

N i 2 M o 3 O 8 : Complex antiferromagnetic order on a honeycomb lattice journal, January 2019

Neutron scattering in the proximate quantum spin liquid α-RuCl 3 journal, June 2017

Ba4[Mn3N6], a Quasi-One-Dimensional Mixed-Valent Nitridomanganate (II, IV) journal, May 2018

Single crystal growth from separated educts and its application to lithium transition-metal oxides journal, October 2016

Pressure-Tuned Interactions in Frustrated Magnets: Pathway to Quantum Spin Liquids? journal, December 2019

Three-dimensional quantum anomalous Hall effect in hyperhoneycomb lattices journal, May 2018

The 2016 oxide electronic materials and oxide interfaces roadmap text, January 2016

Neutron scattering in the proximate quantum spin liquid α-RuCl3. text, January 2017

Three dimensional quantum spin liquids in models of harmonic-honeycomb iridates and phase diagram in an infinite-D approximation text, January 2013

Line of Dirac Nodes in Hyper-Honeycomb Lattices text, January 2014

Weyl spin liquids text, January 2014

Pressure and magnetic-field effects on metal-insulator transitions of bulk and domain-wall states in pyrochlore iridates text, January 2015

Loop-nodal and Point-nodal Semimetals in Three-dimensional Honeycomb Lattices text, January 2015

Recent progress on correlated electron systems with strong spin-orbit coupling text, January 2015

Challenges in Design of Kitaev Materials: Magnetic Interactions from Competing Energy Scales text, January 2016

Low-energy Spin Dynamics of the Honeycomb Spin Liquid Beyond the Kitaev Limit text, January 2016

Kitaev materials beyond iridates: order by quantum disorder and Weyl magnons in rare-earth double perovskites text, January 2016

Uniaxial and hydrostatic pressure effects in alpha-RuCl3 single crystals via thermal-expansion measurements text, January 2017

Spin-orbit coupled systems in the "atomic" limit: rhenates, osmates, iridates text, January 2018

Antiferromagnetic Kitaev Interaction in $f$-Electron Based Honeycomb Magnets text, January 2018

Kitaev-like honeycomb magnets: Global phase behavior and emergent effective models text, January 2019

Heisenberg-Kitaev Models on Hyperhoneycomb and Stripyhoneycomb Lattices: 3D-2D Equivalence of Ordered States and Phase Diagrams text, January 2019

Polarized-neutron investigation of magnetic ordering and spin dynamics in BaCo 2 (AsO 4 ) 2 frustrated honeycomb-lattice magnet journal, January 2018

Erratum: Iridates from the molecular side journal, August 2016

Exactly solvable Kitaev model in three dimensions
journal, January 2009

Competitions in Layered Ruthenates: Ferromagnetism versus Antiferromagnetism and Triplet versus Singlet Pairing
journal, May 1999

NaIrO3—A pentavalent post-perovskite
journal, March 2011

Simple Models of Magnetism
book, January 2008

Zigzag Magnetic Order in the Iridium Oxide ${Na}_{2} {IrO}_{3}$
journal, February 2013

Anyons in an exactly solved model and beyond
journal, January 2006

Mott Insulators in the Strong Spin-Orbit Coupling Limit: From Heisenberg to a Quantum Compass and Kitaev Models
journal, January 2009

Cuprate Superconductivity: Dependence of $T_{c}$ on the $c$ -Axis Layering Structure
journal, July 1999

Absence of Ferromagnetism or Antiferromagnetism in One- or Two-Dimensional Isotropic Heisenberg Models
journal, November 1966

Torque magnetometry in pulsed magnetic fields with use of a commercial microcantilever
journal, August 2002

Physical properties of the n =3 Ruddlesden - Popper compound
journal, November 1998

Kitaev-Heisenberg Model on a Honeycomb Lattice: Possible Exotic Phases in Iridium Oxides $A_{2} {IrO}_{3}$
journal, July 2010

Three-dimensional quantum spin liquids in models of harmonic-honeycomb iridates and phase diagram in an infinite- $D$ approximation
journal, November 2014

Heisenberg-Kitaev model on the hyperhoneycomb lattice
journal, January 2014

Hybrid Improper Ferroelectricity: A Mechanism for Controllable Polarization-Magnetization Coupling
journal, March 2011

Structure and properties of ordered Li2IrO3 and Li2PtO3
journal, August 2008

Magnetic Field-Tuned Quantum Criticality in the Metallic Ruthenate Sr3Ru2O7
journal, October 2001

Experimentally determining the exchange parameters of quasi-two-dimensional Heisenberg magnets
journal, August 2008

Relevance of the Heisenberg-Kitaev Model for the Honeycomb Lattice Iridates $A_{2} {IrO}_{3}$
journal, March 2012

Spin Waves and Revised Crystal Structure of Honeycomb Iridate ${Na}_{2} {IrO}_{3}$
journal, March 2012

Magnetic excitation spectrum of Na $_{2}$ IrO $_{3}$ probed with resonant inelastic x-ray scattering
journal, June 2013

Exactly solvable Kitaev model in three dimensions
text, January 2008

Heisenberg-Kitaev model on hyperhoneycomb lattice
text, January 2013

Three dimensional quantum spin liquids in models of harmonic-honeycomb iridates and phase diagram in an infinite-D approximation
text, January 2013

Anyons in an exactly solved model and beyond
text, January 2005

Ab Initio Approaches for Low‐Energy Spin Hamiltonians
journal, March 2019

Comparative study of monolithic platinum and iridium as oxygen-evolving anodes during the electrolytic reduction of uranium oxide in a molten LiCl–Li2O electrolyte
journal, February 2019

Iridates from the molecular side
journal, July 2016

Raman spectroscopic signature of fractionalized excitations in the harmonic-honeycomb iridates β- and γ-Li2IrO3
journal, July 2016

Proximate Kitaev quantum spin liquid behaviour in a honeycomb magnet
journal, April 2016

Evidence for anionic redox activity in a tridimensional-ordered Li-rich positive electrode β-Li2IrO3
journal, February 2017

Direct evidence for dominant bond-directional interactions in a honeycomb lattice iridate Na2IrO3
journal, May 2015

Correlated states in β-Li2IrO3 driven by applied magnetic fields
journal, October 2017

Theory of the field-revealed Kitaev spin liquid
journal, June 2019

Path to stable quantum spin liquids in spin-orbit coupled correlated materials
journal, April 2018

Concept and realization of Kitaev quantum spin liquids
journal, March 2019

Kitaev exchange and field-induced quantum spin-liquid states in honeycomb α-RuCl3
journal, November 2016

The 2016 oxide electronic materials and oxide interfaces roadmap
journal, October 2016

Recent progress on correlated electron systems with strong spin–orbit coupling
journal, August 2016

Quantum spin liquids: a review
journal, November 2016

Barrier tunneling of the loop-nodal semimetal in the hyperhoneycomb lattice
journal, April 2018

Resonant inelastic x-ray scattering study of $\alpha$ -RuCl ₃ : a progress report
journal, January 2020

The challenge of spin–orbit-tuned ground states in iridates: a key issues review
journal, February 2018

Frustration and quantum criticality
journal, May 2018

Residual entropy and spin fractionalizations in the mixed-spin Kitaev model
journal, September 2019

All-oxide ferromagnetic resonance and spin pumping with $SrIr O_{3}$
journal, September 2019

Lattice dynamics and structural transition of the hyperhoneycomb iridate $β - {Li}_{2} {IrO}_{3}$ investigated by high-pressure Raman scattering
journal, February 2020

Spin dynamics and field-induced magnetic phase transition in the honeycomb Kitaev magnet $α − {Li}_{2} {IrO}_{3}$
journal, February 2019

Universal tensor-network algorithm for any infinite lattice
journal, May 2019

Non-Kitaev spin liquids in Kitaev materials
journal, May 2019

Antiferromagnetic Kitaev interaction in $f$ -electron based honeycomb magnets
journal, June 2019

Hidden Plaquette Order in a Classical Spin Liquid Stabilized by Strong Off-Diagonal Exchange
journal, June 2019

Crystal growth and magnetic anisotropy in the spin-chain ruthenate ${Na}_{2} {RuO}_{4}$
journal, February 2018

$N i_{2} M o_{3} O_{8}$ : Complex antiferromagnetic order on a honeycomb lattice
journal, January 2019

Neutron scattering in the proximate quantum spin liquid α-RuCl ₃
journal, June 2017

Ba4[Mn3N6], a Quasi-One-Dimensional Mixed-Valent Nitridomanganate (II, IV)
journal, May 2018

Single crystal growth from separated educts and its application to lithium transition-metal oxides
journal, October 2016

Pressure-Tuned Interactions in Frustrated Magnets: Pathway to Quantum Spin Liquids?
journal, December 2019

Three-dimensional quantum anomalous Hall effect in hyperhoneycomb lattices
journal, May 2018

The 2016 oxide electronic materials and oxide interfaces roadmap
text, January 2016

Neutron scattering in the proximate quantum spin liquid α-RuCl3.
text, January 2017

Three dimensional quantum spin liquids in models of harmonic-honeycomb iridates and phase diagram in an infinite-D approximation
text, January 2013

Line of Dirac Nodes in Hyper-Honeycomb Lattices
text, January 2014

Weyl spin liquids
text, January 2014

Pressure and magnetic-field effects on metal-insulator transitions of bulk and domain-wall states in pyrochlore iridates
text, January 2015

Loop-nodal and Point-nodal Semimetals in Three-dimensional Honeycomb Lattices
text, January 2015

Recent progress on correlated electron systems with strong spin-orbit coupling
text, January 2015

Challenges in Design of Kitaev Materials: Magnetic Interactions from Competing Energy Scales
text, January 2016

Low-energy Spin Dynamics of the Honeycomb Spin Liquid Beyond the Kitaev Limit
text, January 2016

Kitaev materials beyond iridates: order by quantum disorder and Weyl magnons in rare-earth double perovskites
text, January 2016

Uniaxial and hydrostatic pressure effects in alpha-RuCl3 single crystals via thermal-expansion measurements
text, January 2017

Spin-orbit coupled systems in the "atomic" limit: rhenates, osmates, iridates
text, January 2018

Antiferromagnetic Kitaev Interaction in $f$-Electron Based Honeycomb Magnets
text, January 2018

Kitaev-like honeycomb magnets: Global phase behavior and emergent effective models
text, January 2019

Heisenberg-Kitaev Models on Hyperhoneycomb and Stripyhoneycomb Lattices: 3D-2D Equivalence of Ordered States and Phase Diagrams
text, January 2019

Polarized-neutron investigation of magnetic ordering and spin dynamics in BaCo 2 (AsO 4 ) 2 frustrated honeycomb-lattice magnet
journal, January 2018

Erratum: Iridates from the molecular side
journal, August 2016

Robust spin correlations at high magnetic fields in the harmonic honeycomb iridates
journal, August 2017

Theory of the field-revealed Kitaev spin liquid
journal, June 2019

Ba4[Mn3N6], a Quasi-One-Dimensional Mixed-Valent Nitridomanganate (II, IV)
journal, May 2018