High-field spin-flop state in green dioptase

TL;DR

This study investigates the high-field magnetic behavior of green dioptase, revealing a smooth transition from a Ne9el to a spin-flop state driven by magnetic field, using neutron diffraction and magnetization measurements.

Contribution

It provides the first detailed analysis of the high-field magnetic phase transition in green dioptase, combining experimental data with a theoretical model of coupled antiferromagnetic chains.

Findings

Identified a spin-flop transition at 12.2 T in green dioptase.

Observed a smooth evolution of magnetic structure without change in periodicity.

Modeled the magnetic behavior with ferromagnetically coupled antiferromagnetic chains.

Abstract

The high-field magnetic properties and magnetic order of the gem mineral green dioptase Cu$_6[$Si$_6$O$_{18}]\cdot 6$H$_2$O have been studied by means of single-crystal neutron diffraction in magnetic fields up to $21~$T and magnetization measurements up to $30~$T. In zero field, the Cu$^{2+}$-moments in the antiferromagnetic chains are oriented along the $c$-axis with a small off-axis tilt. For a field applied parallel to the $c$-axis, the magnetization shows a spin-flop-like transition at $B^*=12.2~$T at $1.5~$K. Neutron diffraction experiments show a smooth behavior in the intensities of the magnetic reflections without any change in the periodicity of the magnetic structure. Bulk and microscopic observations are well described by a model of ferromagnetically coupled antiferromagnetic $XXZ$ spin-$\frac{1}{2}$ chains, taking into account a change of the local easy-axis direction. We demonstrate that the magnetic structure evolves smoothly from a deformed N\'eel state at low fields to a deformed spin-flop state in a high field via a strong crossover around $B^*$. The results are generalized for different values of interchain coupling and spin anisotropy.