Characterization of the Spin-1/2 Linear-Chain Ferromagnet CuAs$_2$O$_4$

Abstract

The magnetic and lattice properties of the $S$=1/2 quantum-spin-chain ferromagnet, CuAs$_2$O$_4$, mineral name trippkeite, were investigated. The crystal structure of CuAs$_2$O$_4$ is characterized by the presence of corrugated CuO$_2$ ribbon chains. Measurements of the magnetic susceptibility, heat capacity, electron paramagnetic resonance and Raman spectroscopy were performed. Our experiments conclusively show that a ferromagnetic transition occurs at $\sim$7.4 K. $\textit{Ab initio}$ DFT calculations reveal dominant ferromagnetic nearest-neighbor and weaker antiferromagnetic next- nearest-neighbor spin exchange interactions along the ribbon chains. The ratio of $J_{\rm nn}$/$J_{\rm nnn}$ is near -4, placing CuAs$_2$O$_4$ in close proximity to a quantum critical point in the $J_{\rm nn}$ - $J_{\rm nnn}$ phase diagram. TMRG simulations used to analyze the magnetic susceptibility confirm this ratio. Single-crystal magnetization measurements indicate that a magnetic anisotropy forces the Cu$^{2+}$ spins to lie in an easy plane perpendicular to the $c$-axis. An analysis of the field and temperature dependent magnetization by modified Arrott plots reveals a 3d-XY critical behavior. Lattice perturbations induced by quasi-hydrostatic pressure and temperature were mapped via magnetization and Raman spectroscopy.