Magnetic ground states and excitations in Zn-doped averieite -- a family of oxide-based $S=1/2$ kagome antiferromagnets

Abstract

Spin-1/2 kagome materials have recently attracted a resurgence of interest as they are considered an ideal host of the quantum spin liquid (QSL) state, which can underpin functionality such as superconductivity. Here we report the first synthesis and characterization of a new oxide-based distorted $S=1/2$ kagome antiferromagnet (KAFM) in the Zn${}_x$Cu${}_{5-x}$(VO${}_4$)${}_2$O${}_2$CsCl (termed Zn${}_{\mathbf{x}}$) series, namely Zn${}_2$-averievite, Zn${}_2$ ($x=2$). Using magnetometry, synchrotron diffraction and neutron scattering we demonstrate an evolution of ground states with $x$ in Zn${}_{\mathbf{x}}$; from long-range magnetic order in averievite ($x=0$), via a spin-glass-like ground state in Zn${}_1$, to a quantum spin liquid (QSL) in Zn${}_2$ for which inelastic neutron scattering reveals a gapless continuum of excitations. Similar to archetypal $S=1/2$ KAFMs herbertsmithite and SrCr${}_{8.19}$Ga${}_{3.81}$O${}_{19}$ (SCGO), the dynamic magnetic susceptibility of Zn${}_2$ shows scaling behavior consistent with proximity to a quantum critical point. The results demonstrate that the new Zn${}_2$ material is an excellent test bed for achieving the elusive goal of charge carrier doping in QSL states of $S=1/2$ KAFMs, in-line with previous theoretical studies.

15 pages, 7 figures, Supplemental Material