Effect of Zn doping on the antiferromagnetism in kagome Cu${}_{4-x}$Zn${}_x$(OH)${}_6$FBr

Abstract

Barlowite Cu${}_4$(OH)${}_6$FBr shows three-dimensional (3D) long-range antiferromagnetism, which is fully suppressed in Cu${}_3$Zn(OH)${}_6$FBr with a kagome quantum spin liquid ground state. Here we report systematic studies on the evolution of magnetism in the Cu${}_{4-x}$Zn${}_x$(OH)${}_6$FBr system as a function of $x$ to bridge the two limits of Cu${}_4$(OH)${}_6$FBr ($x$=0) and Cu${}_3$Zn(OH)${}_6$FBr ($x$=1). Neutron-diffraction measurements reveal a hexagonal-to-orthorhombic structural change with decreasing temperature in the $x$ = 0 sample. While confirming the 3D antiferromagnetic nature of low-temperature magnetism, the magnetic moments on some Cu${}^{2+}$ sites on the kagome planes are found to be vanishingly small, suggesting strong frustration already exists in barlowite. Substitution of interlayer Cu${}^{2+}$ with Zn${}^{2+}$ with gradually increasing $x$ completely suppresses the bulk magnetic order at around $x$ = 0.4, but leaves a local secondary magnetic order up to $x\sim 0.8$ with a slight decrease in its transition temperature. The high-temperature magnetic susceptibility and specific heat measurements further suggest that the intrinsic magnetic properties of kagome spin liquid planes may already appear from $x>0.3$ samples. Our results reveal that the Cu${}_{4-x}$Zn${}_x$(OH)${}_6$FBr may be the long-thought experimental playground for the systematic investigations of the quantum phase transition from a long-range antiferromagnet to a topologically ordered quantum spin liquid.

9 pages, 6 figures

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