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Magnetoelectric initialization of multiferroic Mn2GeO4

Naëmi Leo1,2,*, Jonathan S. White3, Michel Kenzelmann3, Takashi Honda4, Tsuyoshi Kimura5, Dennis Meier6,7,8, and Manfred Fiebig1

  • *Contact author: n.leo@lboro.ac.uk

Phys. Rev. B 114, 194407 – Published 13 October, 2026

DOI: https://doi.org/10.1103/qcg2-3y34

Abstract

Magnetoelectric multiferroics promise direct cross control between coexisting ferroelectric and ferromagnetic orders, which is of interest for applications in magnetism and spintronics. A particularly interesting type of cross control is found in spin-spiral multiferroic Mn2GeO4, in which a ferroelectric multidomain distribution can be globally inverted by a single magnetic field sweep. In this work we show that this repeatable response is not obtained immediately after entering the multiferroic phase via zero-field coolling. Instead, an initial metastable multidomain state forms in which polarization, magnetization, and antiferromagnetic order do not yet minimize the trilinear magnetoelectric coupling. Using optical second-harmonic generation for ferroelectric domain imaging, we demonstrate that a single field cycle deterministically drives the system from the initial metastable state into an equilibrium domain configuration that shows repeatable domain interconversion. This initialization behavior originates from a deterministic pathway from metastable to equilibrium domain patterns, in contrast to the more common—and less reliable—stochastic domain “training” procedures that require repeated field cycles. Understanding the initial domain evolution thus enables reliable cross control in magnetoelectric devices with highly interlinked order parameters.

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