Selective doping Barlowite for quantum spin liquid: a first-principles study

Abstract

Barlowite $C{u}_4(OH{)}_{6}FBr$ is a newly found mineral containing $C{u}^{2+}$ kagome planes. Despite similarities in many aspects to Herbertsmithite $C{u}_{3}Zn(OH{)}_{6}C{l}_2$, the well-known quantum spin liquid (QSL) candidate, intrinsic Barlowite turns out not to be a QSL, possibly due to the presence of $C{u}^{2+}$ ions in between kagome planes that induce interkagome magnetic interaction [PRL, 113, 227203 (2014)]. Using first-principles calculation, we systematically study the feasibility of selective substitution of the interkagome Cu ions with isovalent nonmagnetic ions. Unlike previous speculation of using larger dopants, such as $C{d}^{2+}$ and $C{a}^{2+}$, we identify the most ideal stoichiometric doping elements to be Mg and Zn in forming $C{u}_{3}Mg(OH{)}_{6}FBr$ and $C{u}_{3}Zn(OH{)}_{6}FBr$ with the highest site selectivity and smallest lattice distortion. The equilibirium anti-site disorder in Mg/Zn- doped Barlowite is estimated to be one order of magnitude lower than that in Herbertsmithite. The single-electron band structure and orbital component analysis show that the proposed selective doping effectively mitigates the difference between Barlowite and Herbertsmithite.

5 pages, 3 figures

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Cited by in corpus (21)

• The Chemistry of Quantum Spin Liquids
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• Quantum Magnetism in Minerals
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• 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
• Dynamic fingerprint of fractionalized excitations in single-crystalline Cu${}_3$Zn(OH)${}_6$FBr
• 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
• Synthesis-Dependent Properties of Barlowite and Zn-Substituted Barlowite
• Doping quantum spin liquids on the Kagome lattice
• Site-Specific Structure at Multiple Length Scales in Kagome Quantum Spin Liquid Candidates
• Nuclear and Magnetic Structures of the Frustrated Quantum Antiferromagnet Barlowite, Cu${}_4$(OH)${}_6$FBr
• Magnetic resonance as a local probe for kagomé magnetism in Barlowite Cu${}_4$(OH)${}_6$FBr
• Classical and quantum order in hyperkagome antiferromagnets
• Antiferromagnetism in kagome $\alpha$-Cu${}_3$Mg(OH)${}_6$Br${}_2$
• 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
• Distinguishing thermodynamics and spectroscopy for octupolar U(1) spin liquid of Ce-pyrochlores
• Magnetically ordered and kagome quantum spin liquid states in the Zn-doped claringbullite series
• Li doping kagome spin liquid compounds
• Combinatorial exploration of quantum spin liquid candidates in the herbertsmithite material family
• Electron-Nuclear Hyperfine Coupling in Quantum Kagome Antiferromagnets from First-Principles Calculation and a Reflection of the Defect Effect