Resolving the local distortions of Ising-like moments in magnetoelectric Ho-doped langasite

TL;DR

This study combines neutron diffraction and magnetization experiments to resolve local distortions of Ho$^{3+}$ magnetic moments in magnetoelectric langasite, revealing complex magnetic configurations influenced by local symmetry breaking.

Contribution

It introduces a model for field-induced magnetic configurations considering local distortions and symmetry operations, advancing understanding of magnetic behavior in Ho-doped langasite.

Findings

Local distortions of Ho$^{3+}$ moments are characterized.

A model for magnetic configurations with arbitrary Ising axis orientations is proposed.

Local susceptibility tensors deviate from pure Ising behavior at low fields.

Abstract

The magnetic properties of Ho-doped langasites (La:Ho)$_3$Ga$_5$SiO$_{14}$ are dominated by the Ising-like magnetic moments of the Ho$^{3+}$ ions. In their saturated regime, the induced magnetic state breaks both time and space inversion symmetries, leading to a novel linear magnetoelectric effect. However, due to distortions induced by a shared Ga/Si occupancy of the 2d sites, resolving the microscopic nature of the magnetic configuration remains a difficult task. Here we combine polarized neutron diffraction and angular dependent magnetization experiments to determine the local distortions of the Ho$^{3+}$ magnetic moments in doped langasites (La$_{1-x}$Ho$_x$)$_3$Ga$_5$SiO$_{14}$ with $x \approx 0.015$ and $x \approx 0.045$. We propose a model for a field-induced magnetic configuration with arbitrary orientations of the local Ising axis of Ho$^{3+}$ in distorted positions. The operations of broken local $C_2$ symmetry and rotations around the trigonal $C_3$ axis connect different sites, restoring the global P321 symmetry of the crystal and simplifying the description of the magnetic properties. The superposition of two distorted Ho$^{3+}$ positions connected by $C_2$ symmetry determines the local magnetic susceptibility tensor, which no longer appears Ising-like at low fields.