Materializing Rival Ground States in the Barlowite Family of Kagome Magnets: Quantum Spin Liquid, Spin Ordered, and Valence Bond Crystal States

Abstract

The spin-$\frac{1}{2}$ kagome antiferromagnet is considered an ideal host for a quantum spin liquid ground state. We find that when the bonds of the kagome lattice are modulated with a periodic pattern, new quantum ground states emerge. Newly synthesized crystalline barlowite (Cu${}_4$(OH)${}_6$FBr) and Zn-substituted barlowite demonstrate the delicate interplay between singlet states and spin order on the spin-$\frac{1}{2}$ kagome lattice. Comprehensive structural measurements demonstrate that our new variant of barlowite maintains hexagonal symmetry at low temperatures with an arrangement of distorted and undistorted kagome triangles, for which numerical simulations predict a pinwheel valence bond crystal (VBC) state instead of a quantum spin liquid (QSL). The presence of interlayer spins eventually leads to an interesting pinwheel $q=0$ magnetic order. Partially Zn-substituted barlowite (Cu${}_{3.44}$Zn${}_{0.56}$(OH)${}_6$FBr) has an ideal kagome lattice and shows QSL behavior, indicating a surprising robustness of the QSL against interlayer impurities. The magnetic susceptibility is similar to that of herbertsmithite, even though the Cu${}^{2+}$ impurities are above the percolation threshold for the interlayer lattice and they couple more strongly to the nearest kagome moment. This system is a unique playground displaying QSL, VBC, and spin order, furthering our understanding of these highly competitive quantum states.

arXiv comment31 pages, 7 figures

References in corpus (40)

• Quantum Spin Liquids
• Spin Liquid Ground State of the $S=1/2$ Kagome Heisenberg Model
• Fractionalized excitations in the spin liquid state of a kagomé lattice antiferromagnet
• Spin Dynamics of the Spin-1/2 Kagome Lattice Antiferromagnet ZnCu_3(OH)_6Cl_2
• Identifying Topological Order by Entanglement Entropy
• Projected wavefunction study of Spin-1/2 Heisenberg model on the Kagome lattice
• Herbertsmithite and the Search for the Quantum Spin Liquid
• Gapless spin-liquid ground state in the $S=1/2$ kagome antiferromagnet
• Evidence for a Gapped Spin-Liquid Ground State in a Kagome Heisenberg Antiferromagnet
• Properties of an algebraic spin liquid on the kagome lattice
• Ground State of the Kagome Lattice Heisenberg Antiferromagnet
• Dirac, Anderson, and Goldstone on the Kagome
• Bond and Site Percolation in Three Dimensions
• Physics of low energy singlet states of the Kagome lattice quantum Heisenberg antiferromagnet
• Correlated impurities and intrinsic spin liquid physics in the kagome material Herbertsmithite
• Gapped spin-1/2 spinon excitations in a new kagome quantum spin liquid compound Cu${}_3$Zn(OH)${}_6$FBr
• Gapped spin liquid with ${\mathbb{Z}}_2$-topological order for kagome Heisenberg model
• Low temperature magnetization of the S=1/2 kagome antiferromagnet ZnCu_3(OH)_6Cl_2
• Pinwheel VBS state and triplet excitations in the two-dimensional deformed kagome lattice
• First-principles determination of Heisenberg Hamiltonian parameters for the spin-1/2 kagome antiferromagnet ZnCu3(OH)6Cl2
• A Schwinger-boson approach to the kagome with Dzyaloshinskii-Moriya interactions: phase diagram and dynamical structure factors
• Refining the Spin Hamiltonian in the Spin-1/2 Kagome Lattice Antiferromagnet ZnCu${}_3$(OH)${}_6$Cl${}_2$ using Single Crystals
• Barlowite: A Spin-1/2 Antiferromagnet with a Geometrically Perfect Kagome Motif
• 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${}_2$
• Renormalization group analysis of competing quantum phases in the J1-J2 Heisenberg model on the kagome lattice
• Hidden long range order in Heisenberg Kagome antiferromagnets
• Quantum criticality of the kagome antiferromagnet with Dzyaloshinskii-Moriya interactions
• Barlowite as a canted antiferromagnet: theory and experiment
• From Claringbullite to a new spin liquid candidate Cu${}_3$Zn(OH)${}_6$FCl
• Single crystal growth of Cu4(OH)6BrF and universal behavior in quantum spin liquid candidates synthetic barlowite and herbertsmithite
• Reduction of magnetic interlayer coupling in barlowite through isoelectronic substitution
• Chiral and Critical Spin Liquids in Spin-$1/2$ Kagome Antiferromagnet
• Effect of Zn doping on the antiferromagnetism in kagome Cu${}_{4-x}$Zn${}_x$(OH)${}_6$FBr
• Striped spin liquid crystal ground state instability of kagome antiferromagnets
• Selective doping Barlowite for quantum spin liquid: a first-principles study
• X-ray Scattering Study of the spin-Peierls transition and soft phonon behavior in TiOCl
• Synthesis-Dependent Properties of Barlowite and Zn-Substituted Barlowite
• External magnetic field effects on a distorted kagome antiferromagnet
• Nuclear and Magnetic Structures of the Frustrated Quantum Antiferromagnet Barlowite, Cu${}_4$(OH)${}_6$FBr
• Spin-1/2 Heisenberg antiferromanget on kagome: a $Z_2$ spin liquid with fermionic spinons

Cited by in corpus (22)

• The Chemistry of Quantum Spin Liquids
• Possible Dirac quantum spin liquid in a kagome quantum antiferromagnet YCu${}_3$(OH)${}_6$Br${}_2$[Br${}_x$(OH)${}_{1-x}$]
• Experimental signatures of quantum and topological states in frustrated magnetism
• Emergence of spin singlets with inhomogeneous gaps in the kagome Heisenberg antiferromagnets Zn-barlowite and herbertsmithite
• From magnetic order to quantum disorder: a $\mu$SR study of the Zn-barlowite series of $S=\frac{1}{2}$ kagomé antiferromagnets, Zn${}_x$Cu${}_{4-x}$(OH)${}_6$FBr
• Doping quantum spin liquids on the Kagome lattice
• Site-Specific Structure at Multiple Length Scales in Kagome Quantum Spin Liquid Candidates
• Controlling frustrated magnetism on the kagome lattice by uniaxial-strain tuning
• Valence bond solid and possible deconfined quantum criticality in an extended kagome lattice Heisenberg antiferromagnet
• Freezing of the Lattice in the Kagome Lattice Heisenberg Antiferromagnet Zn-barlowite ZnCu${}_3$(OD)${}_6$FBr
• Magnetic phase diagram of Cu${}_{4-x}$Zn${}_x$(OH)${}_6$FBr studied by neutron-diffraction and $\mu$SR techniques
• Emergence of the spin polarized domains in the kagome lattice Heisenberg antiferromagnet Zn-barlowite (Zn${}_{0.95}$Cu${}_{0.05}$)Cu${}_3$(OD)${}_6$FBr
• Quantum Phases of Kagome Electron System with Half-Filled Flat Bands
• High energy spin excitations in the quantum spin liquid candidate Zn-barlowite probed by resonant inelastic x-ray scattering
• Chiral Broken Symmetry Descendants of the Kagomé Lattice Chiral Spin Liquid
• Magnetically ordered and kagome quantum spin liquid states in the Zn-doped claringbullite series
• Combinatorial exploration of quantum spin liquid candidates in the herbertsmithite material family
• Valence-Bond Solid phases in the spin-$1/2$ Kekule-Heisenberg model
• Fluctuating magnetism in Zn-doped averievite with well-separated kagome layers
• Pressure-tuned spin chains in brochantite, Cu${}_4$SO${}_4$(OH)${}_6$
• Magnetosynthesis effect on the structure and ground state of Cu${}^{2+}$-based antiferromagnets
• Local probe investigation of the spin dynamics in the kagome and inter-layers of orthorhombic barlowite Cu${}_4$(OD)${}_6$FBr: ${}^{79}$Br and ${}^{63}$Cu NQR study