The Chemistry of Quantum Spin Liquids

Abstract

Quantum spin liquids are an exciting playground for exotic physical phenomena and emergent many-body quantum states. The realization and discovery of quantum spin liquid candidate materials and associated phenomena lie at the intersection of solid-state chemistry, condensed matter physics and materials science and engineering. In this review, we provide the current status of the crystal chemistry, synthetic techniques, physical properties, and research methods in the field of quantum spin liquids. We also highlight a number of specific quantum spin liquid candidate materials and their structure-property relationships, elucidating their fascinating behavior and connecting it to the intricacies of their structures. Furthermore, we share our thoughts on defects and their inevitable presence in materials, of which quantum spin liquids are no exception, which can complicate the interpretation of characterization of these materials, and urge the community to extend their attention to materials preparation and data analysis, cognizant of the impact of defects. This review was written with the intention of providing guidance on improving the materials design and growth of quantum spin liquids, and painting a picture of the beauty of the underlying chemistry of this exciting class of materials.

Submitted for publication in a special issue on quantum materials in Chemical Reviews. Open for comment, please provide suggestions for additional references and improvements

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• Giant anomalous Nernst effect in the magnetic Weyl semimetal Co3Sn2S2
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• Lightly stuffed pyrochlore structure of single-crystalline Yb2Ti2O7 grown by the optical floating zone technique
• Order in the Heisenberg Pyrochlore: The Magnetic Structure of Gd2Ti2O7
• Dynamic Scaling in the Susceptibility of the Spin-1\2 Kagome Lattice Antiferromagnet Herbertsmithite
• Quantum Spin Ice Dynamics in the Dipole-Octupole Pyrochlore Magnet Ce${}_2$Zr${}_2$O${}_7$
• Scale-free antiferromagnetic fluctuations in the S=1/2 kagome antiferromagnet herbertsmithite
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• Importance of anisotropic exchange interactions in honeycomb iridates. Minimal model for zigzag antiferromagnetic order in Na${}_2$IrO${}_3$
• Specific Heat of Kagome Ice in the Pyrochlore Oxide Dy2Ti2O7
• Thermal conductivity and specific heat of the linear chain cuprate Sr${}_2$CuO${}_3$: Evidence for thermal transport via spinons
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• Low temperature magnetization of the S=1/2 kagome antiferromagnet ZnCu_3(OH)_6Cl_2
• Rethinking $\alpha$-RuCl${}_3$
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• Is the Yb2Ti2O7 pyrochlore a quantum spin ice?
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• Sliding Density-Wave in Sr_{14}Cu_{24}O_{41} Ladder Compounds
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• Evidence for a three-dimensional quantum spin liquid in PbCuTe${}_2$O${}_6$
• Strong quantum fluctuations in a quantum spin liquid candidate with a Co-based triangular lattice
• Vacancy defects and monopole dynamics in oxygen-deficient pyrochlores
• Stuffed Rare Earth Pyrochlore Solid Solutions
• Experimental signatures of emergent quantum electrodynamics in Pr${}_2$Hf${}_2$O${}_7$
• Gapless excitations in the ground state of 1T-TaS${}_2$
• Refining the Spin Hamiltonian in the Spin-1/2 Kagome Lattice Antiferromagnet ZnCu${}_3$(OH)${}_6$Cl${}_2$ using Single Crystals
• Spin Waves and Quantum Criticality in the Frustrated XY Pyrochlore Antiferromagnet Er2Ti2O7
• Quantum spin liquids in frustrated spin-1 diamond antiferromagnets
• Structural Fluctuations in the Spin Liquid State of Tb2Ti2O7
• Removing the spin ice cap: magnetic ground states of rare earth tripod kagome lattice Mg${}_2$RE${}_3$Sb${}_3$O${}_{14}$ (RE = Gd, Dy, Er)
• Magnetic excitations in coupled Haldane spin chains near the quantum critical point
• Quantum and Classical Phases of the Pyrochlore Heisenberg Model with Competing Interactions
• Bond disordered spin liquid and the honeycomb iridate H${}_3$LiIr${}_2$O${}_6$ $-$ abundant low energy density of states from random Majorana hopping
• Barlowite: A Spin-1/2 Antiferromagnet with a Geometrically Perfect Kagome Motif
• Emergent Order in the Kagome Ising Magnet Dy3Mg2Sb3O14
• Synthesis and Characterization of Single Crystal Samples of Spin-$1/2$ Kagome Lattice Antiferromagnets in the Zn-Paratacamite Family Zn${}_x$Cu${}_{4-x}$(OH)${}_6$Cl${}_2$
• Magnetic properties and heat capacity of the three-dimensional frustrated S=1/2 antiferromagnet PbCuTe2O6
• Impact of Stoichiometry of Yb2Ti2O7 on its Physical Properties
• Magnetic order in single crystals of Na3Co2SbO6 with a honeycomb arrangement of 3d${}^7$ Co${}^{2+}$ ions
• Molecular Quantum Magnetism in LiZn2Mo3O8
• High pressure floating-zone growth of perovskite nickelate LaNiO3 single crystals
• Field-Induced Magnetic Order in Quantum Spin Liquids
• Spin Liquid State in the 3D Frustrated Antiferromagnet PbCuTe2O6: NMR and muSR Studies
• Magnetic thermal conductivity far above the Néel temperatures in the Kitaev-magnet candidate $\alpha$-RuCl${}_3$
• Spin dynamics and spin freezing behavior in the two-dimensional antiferromagnet NiGa${}_2$S${}_4$ revealed by Ga-NMR, NQR and $\mu$SR measurements
• High oxygen pressure floating zone growth and crystal structure of the layered nickelates R${}_4$Ni${}_3$O${}_{10}$ (R=La, Pr)
• Tunable Magnetic Transition to a Singlet Ground State in a 2D Van der Waals Layered Trimerized Kagomé Magnet
• Direct observation of multi-spinon excitations outside of the two-spinon continuum in the antiferromagnetic spin chain cuprate Sr2CuO3
• Breathing chromium spinels: a showcase for a variety of pyrochlore Heisenberg Hamiltonians
• Fractionalized excitations in the partially magnetized spin liquid candidate YbMgGaO4
• Candidate quantum spin ice in the pyrochlore Pr${}_2$Hf${}_2$O${}_7$
• Zero-field incommensurate spin-Peierls phase with interchain frustration in TiOCl
• Single crystal growth from separated educts and its application to lithium transition-metal oxides
• Energetic selection of ordered states in a model of the Er2Ti2O7 frustrated pyrochlore XY antiferromagnet
• From Spin Glass to Quantum Spin Liquid Ground States in Molybdate Pyrochlores
• Gapless quantum excitations from an Ice-like Splayed Ferromagnetic ground state in stoichiometric Yb2Ti2O7
• Synthesis, floating zone crystal growth and characterization of the Quantum Spin Ice $\mathrm{P}{\mathrm{r}}_2\mathrm{Z}{\mathrm{r}}_2{\mathrm{O}}_7$ pyrochlore
• Spin-orbital Entangled Molecular $j_{\mathrm{eff}}$ States in Lacunar Spinel Compounds
• Rearrangement of Van-der-Waals Stacking and Formation of a Singlet State at $T=90$ K in a Cluster Magnet
• Scalar Chiral Spin-1/2 Order on Kagome Lattices in Nd3Sb3Mg2O14
• Lattice-Tuned Magnetism of Ru4+(4d4) Ions in Single-Crystals of the Layered Honeycomb Ruthenates: Li2RuO3 and Na2RuO3
• Symmetry Reduction in the Quantum Kagome Antiferromagnet Herbertsmithite
• Weak ferromagnetism of quasi-one-dimensional S=1/2 antiferromagnet BaCu${}_2$Ge${}_2$O${}_7$
• Field Induced Magnetic Ordering and Single-ion Anisotropy in the Quasi-1D Haldane Chain Compound SrNi2V2O8: A Single Crystal investigation
• Heat transport study of the spin liquid candidate 1T-TaS2
• Local magnetism and spin correlations in the geometrically frustrated cluster magnet LiZn${}_2$Mo${}_3$O${}_8$
• Field-induced intertwined orders in 3D Mott-Kitaev honeycomb $\beta$-Li2IrO3
• Signatures of a gearwheel quantum spin liquid in a spin-$\frac{1}{2}$ pyrochlore molybdate Heisenberg antiferromagnet
• Emergent honeycomb lattice in LiZn2Mo3O8
• Quantum spin fluctuations in the spin liquid state of Tb2Ti2O7
• Spin liquid close to a quantum critical point in Na${}_4$Ir${}_3$O${}_8$
• Local Spin Susceptibility of the S=1/2 Kagome Lattice in ZnCu3(OD)6Cl2
• Quantum Spin Liquid in a Breathing Kagome Lattice
• Stability of the spiral spin liquid in MnSc${}_2$S${}_4$
• Materializing Rival Ground States in the Barlowite Family of Kagome Magnets: Quantum Spin Liquid, Spin Ordered, and Valence Bond Crystal States
• Mott Transition and Superconductivity in Quantum Spin Liquid Candidate NaYbSe${}_2$
• Quantum spin ice on the breathing pyrochlore lattice
• Orbitally induced hierarchy of exchange interactions in zigzag antiferromagnetic state of honeycomb silver delafossite Ag3Co2SbO6
• CuSiO_3 : a quasi - one - dimensional S=1/2 antiferromagnetic chain system
• Low Temperature Specific Heat of Dy${}_2$Ti${}_2$O${}_7$ in the Kagome Ice State
• Laser-diode-heated floating zone (LDFZ) method appropriate to crystal growth of incongruently melting materials
• Single crystal growth of Cu4(OH)6BrF and universal behavior in quantum spin liquid candidates synthetic barlowite and herbertsmithite
• Topological Paramagnetism in Frustrated Spin-One Mott Insulators
• Vesignieite: a $S=\frac{1}{2}$ kagome antiferromagnet with dominant third-neighbor exchange
• Ground-state selection and spin-liquid behaviour in the classical Heisenberg model on the breathing pyrochlore lattice
• A Supercooled Spin Liquid State in the Frustrated Pyrochlore Dy2Ti2O7
• Frustrated Spin One On A Diamond Lattice
• Absence of Jahn-Teller transition in the hexagonal Ba3CuSb2O9 single crystal
• Electron Spin Resonance on the spin-1/2 triangular magnet NaYbS2
• Emergent orbitals in the cluster Mott insulator on a breathing Kagome lattice
• New Honeycomb Iridium (V) Oxides: NaIrO${}_3$ and Sr${}_3$CaIr${}_2$O${}_9$
• Effect of Zn doping on the antiferromagnetism in kagome Cu${}_{4-x}$Zn${}_x$(OH)${}_6$FBr
• Spin-Peierls transition in TiPO${}_4$
• Direct experimental observation of the molecular Jeff=3/2 ground state in the lacunar spinel GaTa4Se8
• NaSrMn2F7, NaCaFe2F7, and NaSrFe2F7: novel single crystal pyrochlore antiferromagnets
• Selective doping Barlowite for quantum spin liquid: a first-principles study
• Synthesis-Dependent Properties of Barlowite and Zn-Substituted Barlowite
• RKKY oscillations in the spin relaxation rates of atomic scale nanomagnets
• Electron doping of proposed quantum spin liquid kagomé Zn-Cu hydroxyl-halides produces localized states in the band gap
• Averievite: a copper oxide kagome antiferromagnet
• Quantum versus Classical Spin Fragmentation in Dipolar Kagome Ice Ho3Mg2Sb3O14
• Disorder driven spin-orbital liquid behaviour in the Ba${}_3$XSb${}_2$O${}_9$ materials
• Quantum Paramagnet and Frustrated Quantum Criticality in a Spin-One Diamond Lattice Antiferromagnet
• The Spin Liquid State of the Tb2Ti2O7 Pyrochlore Antiferromagnet: A Puzzling State of Affairs
• Assessing exchange-correlation functional performance in the chalcogenide lacunar spinels GaM${}_4$Q${}_8$ (M = Mo, V, Nb, Ta; Q = S, Se)
• Magnetic Raman continuum in single crystalline H${}_3$LiIr${}_2$O${}_6$
• Novel magnetism on a honeycomb lattice in a-RuCl3 studied by muon spin rotation
• Antiferromagnetic and Orbital Ordering on a Diamond Lattice Near Quantum Criticality
• The trimer-based spin liquid candidate Ba4NbIr3O12
• Spin--lattice coupling and the emergence of the trimerized phase in the $S=1$ Kagome antiferromagnet Na${}_2$Ti${}_3$Cl${}_8$
• Spinon Excitations in the Quasi-1D S = 1/2 Chain Cs4CuSb2Cl12
• Crystal Field Excitations in Breathing Pyrochlore Antiferromagnet Ba3Yb2Zn5O11
• Orbital Arrangements and Magnetic Interactions in the Quasi-One-Dimensional Cuprates ACuMoO_4(OH) (A = Na, K)
• Double-layered monopolar order in Tb2Ti2O7 spin liquid
• The pyrochlore Ho2Ti2O7: Synthesis, crystal growth and stoichiometry
• Crystal Field Levels and Magnetic Anisotropy in the Kagome Compounds $\mathrm{N}{\mathrm{d}}_3\mathrm{S}{\mathrm{b}}_3\mathrm{M}{\mathrm{g}}_2{\mathrm{O}}_{14}$, $\mathrm{N}{\mathrm{d}}_3\mathrm{S}{\mathrm{b}}_3\mathrm{Z}{\mathrm{n}}_2{\mathrm{O}}_{14}$, and $\mathrm{P}{\mathrm{r}}_3\mathrm{S}{\mathrm{b}}_3\mathrm{M}{\mathrm{g}}_2{\mathrm{O}}_{14}$
• Electronic tunability of the frustrated triangular-lattice cluster magnet LiZn${}_{2-x}$Mo${}_3$O${}_8$
• The Curious Case of NiRh${}_2$O${}_4$: A Spin-Orbit Entangled Diamond Lattice Paramagnet
• Persistent spin dynamics in the pressurized spin-liquid candidate YbMgGaO${}_4$
• Glassy freezing of orbital dynamics in FeCr2S4 and FeSc2S4
• NMR, magnetization, and heat capacity studies of the uniform spin-1/2 chain compound Bi6V3O16
• Growth and Characterization of Iron Scandium Sulfide (FeSc2S4)
• Spin-Orbital Entangled Liquid State in the Copper Oxide Ba${}_3$CuSb${}_2$O${}_9$
• Structure, magnetic susceptibility and specific heat of the spin-orbital-liquid candidate FeSc2S4 : Influence of fe off-stoichiometry
• Controlling the stoichiometry of the triangular lattice antiferromagnet Li${}_{1+x}$Zn${}_{2-y}$Mo${}_3$O${}_8$
• Homogenous reduced moment in a gapful scalar chiral kagome antiferromagnet
• Anisotropic Field-Induced Gap in Quasi-One-Dimensional Antiferromagnet KCuMoO${}_4$(OH)

Cited by in corpus (51)

• Hexagonal Perovskites as Quantum Materials
• Quantum-centric Supercomputing for Materials Science: A Perspective on Challenges and Future Directions
• Molecular Quantum Materials: Electronic Phases and Charge Dynamics in Two-Dimensional Organic Solids
• Experimental signatures of quantum and topological states in frustrated magnetism
• LiYbSe2: Frustrated Magnetism in a New Pyrochlore Lattice
• Ln2(SeO3)2(SO4)(H2O)2 (Ln = Sm, Dy, Yb): A Mixed-Ligand Pathway to New Lathanide (III) Multifunctional Materials Featuring Nonlinear Optical and Magnetic Anisotropy Properties
• From spin liquid to magnetic ordering in the anisotropic kagome Y-Kapellasite Y3Cu9(OH)19Cl8: a single crystal study
• Eminuscent phase in frustrated magnets: a challenge to quantum spin liquids
• A Candidate for the Quantum Spin Liquid Ground-State in the Shastry-Sutherland Lattice Material Yb${}_2$Be${}_2$GeO${}_7$
• Magnetic phase diagram of the breathing-kagome antiferromagnet Nd${}_3$BWO${}_9$
• Site-selective $d^{10}$/$d^0$ substitution in a $S=1/2$ spin ladder Ba${}_2$CuTe${}_{1-x}$W${}_x$O${}_6$ ($0\le x\le 0.3$)
• Quantum critical spin-liquid-like behavior in S = 1/2 quasikagome lattice CeRh1-xPdxSn investigated using muon spin relaxation and neutron scattering
• Role of alkaline metal in the rare-earth triangular antiferromagnet KYbO${}_2$
• Chiral Broken Symmetry Descendants of the Kagomé Lattice Chiral Spin Liquid
• Antiferromagnetic Order in the Rare Earth Halide Perovskites CsEuBr${}_3$ and CsEuCl${}_3$
• First-principles characterization of the magnetic properties of Cu${}_2$(OH)${}_3$Br
• Ferromagnetic Cr4PtGa17: A Novel Half-Heusler-Type Compound with a Breathing Pyrochlore Lattice
• Structure, spin correlations and magnetism of the $S=1/2$ square-lattice antiferromagnet Sr${}_2$CuTe${}_{1-x}$W${}_x$O${}_6$ ($0\le x\le 1$)
• Cascade of phase transitions and large magnetic anisotropy in a triangle-kagome-triangle trilayer antiferromagnet
• Short-range order and hidden energy scale in geometrically frustrated magnets
• Pyrochlore NaYbO2: A potential Quantum Spin Liquid Candidate
• Anomalously field-susceptible spin soft-matter emerging in an electric-dipole liquid candidate
• Magnetic order in the $S_{\mathrm{eff}}$ = 1/2 triangular-lattice compound NdCd${}_3$P${}_3$
• Suppression of the antiferromagnetic order by Zn doping in a possible Kitaev material Na${}_2$Co${}_2$TeO${}_6$
• Structural Modulation and Enhanced Magnetic Ordering in Incommensurate K${}_{1-x}$CrSe${}_2$ Crystals
• Emergent Gauge Fields in Band Insulators
• Honeycomb Layered Frameworks with Metallophilic Bilayers
• Revisiting spin ice physics in the ferromagnetic Ising pyrochlore Pr${}_2$Sn${}_2$O${}_7$
• Widely Spaced Planes of Magnetic Dimers in the Ba6Y2Rh2Ti2O17-δ Hexagonal Perovskite
• Chemo-Structural Disorder in the kagomé spin $S$ = 1/2 systems ZnCu${}_3$(OH)${}_6$Cl${}_2$ and YCu${}_3$(OH)${}_6$Br${}_2$[Br${}_x$(OH)${}_{1-x}$]
• Noncentrosymmetric Triangular Magnet CaMnTeO${}_6$: Strong Quantum Fluctuations and Role of s0 vs. s2 Electronic States in Competing Exchange Interactions
• Modified large-$N$ approach to gapless spin liquids, magnetic orders, and dynamics: Application to triangular lattice antiferromagnets
• Interleaved bond frustration in a triangular lattice antiferromagnet
• High-fidelity dimer excitations using quantum hardware
• Signatures of a gapless quantum spin liquid in the Kitaev material Na${}_3$Co${}_{2-x}$Zn${}_x$SbO${}_6$
• Magnetically disordered ground state in the triangular-lattice antiferromagnets Rb${}_3$Yb(VO${}_4$)${}_2$ and Cs${}_3$Yb(VO${}_4$)${}_2$
• Stoichiometry and Phase Control in K${}_{1-x}$CrSe${}_2$ via Self-Flux Synthesis
• Exactly solvable dissipative dynamics and one-form strong-to-weak spontaneous symmetry breaking in interacting two-dimensional spin systems
• Integer vs. half-integer spin on an approximate honeycomb lattice
• Characterizing the diffuse continuum excitations in the classical spin liquid $h$-YMnO${}_3$
• Keldysh pseudo-fermion functional renormalization group for quantum magnetism
• Hidden frustration in the triangular-lattice antiferromagnet NdCd3P3
• Exerting chemical pressure on the kagome lattice as frustration control in the kapellasite family $A$Cu${}_3$(OH)${}_{6+x}$(Cl,Br)${}_{3-x}$
• Evolution from Topological Dirac Metal to Flat-band-Induced Antiferromagnet in Layered KxNi4S2 (0<=x<=1)
• Spin disorder state induced by Mg${}^{2+}$ doping in a Kitaev material Na${}_3$Co${}_2$SbO${}_6$
• Universal fluctuating regime in triangular chromate antiferromagnets
• Doping dependence of the magnetic ground state in the frustrated magnets Ba${}_2$$M$Te${}_{1-x}$W${}_x$O${}_6$ ($M$ = Mn, Co)
• Coincidence detection techniques for direct measurement of many-body correlations in strongly correlated electron systems
• Quantum spin liquids bootstrapped from Ising criticality in Rydberg arrays
• Stabilizing Itinerant Electrons in a Corner-Sharing Kagomé Oxide Nd4Os3ZnO14
• Bulk magnetic properties of distorted square lattice compounds M'-LnTaO4 (Ln = Tb, Dy, Ho, Er)