Magnetic structure and Dzyaloshinskii-Moriya interaction in the $S=1/2$ helical-honeycomb antiferromagnet $\alpha$-Cu${}_2$V${}_2$O${}_7$

Abstract

Magnetic properties of the $S=1/2$ antiferromagnet $\alpha$-Cu${}_2$V${}_2$O${}_7$ have been studied using magnetization, Quantum Monte Carlo (QMC) simulations, and neutron diffraction. Magnetic susceptibility shows a broad peak at $\sim 50$~K followed by an abrupt increase indicative of a phase transition to a magnetically ordered state at $T_N$ = 33.4(1) K. Above $T_N$, a fit to the Curie-Weiss law gives a Curie-Weiss temperature of $\Theta =-73(1)$~K suggesting the dominant antiferromagnetic coupling. The result of the QMC calculations on the helical-honeycomb spin network with two antiferromagnetic exchange interactions $J_1$ and $J_2$ provides a better fit to the susceptibility than the previously proposed spin-chain model. Two sets of the coupling parameters $J_1:J_2=1:0.45$ with $J_1=5.79(1)$~meV and $0.65:1$ with $J_2=6.31(1)$~meV yield equally good fits down to $\sim T_N$. Below $T_N$, weak ferromagnetism due to spin canting is observed. The canting is caused by the Dzyaloshinskii-Moriya interaction with an estimated $bc$-plane component $\left|D_p\right|$ $\simeq 0.14J_1$. Neutron diffraction reveals that the $S=1/2$ Cu${}^{2+}$ spins antiferromagnetically align in the $F{d}^{\prime }{d}^{\prime }2$ magnetic space group. The ordered moment of 0.93(9)~${\mu }_B$ is predominantly along the crystallographic $a$-axis.

11 pages, 9 figures

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