Abstract

Despite remarkable progress in developing multifunctional materials, spin-driven ferroelectrics featuring both spontaneous magnetization and electric polarization are still rare. Among such ferromagnetic ferroelectrics are conical spin spiral magnets with a simultaneous reversal of magnetization and electric polarization that is still little understood. Such materials can feature various multiferroic domains that complicates their study. Here we study the multiferroic domains in ferromagnetic ferroelectric Mn2GeO4 using neutron diffraction, and show that it features a double-Q conical magnetic structure that, apart from trivial 180o commensurate magnetic domains, can be described by ferromagnetic and ferroelectric domains only. We show unconventional magnetoelectric couplings such as the magnetic-field-driven reversal of ferroelectric polarization with no change of spin-helicity, and present a phenomenological theory that successfully explains the magnetoelectric coupling. Our measurements establish Mn2GeO4 as a conceptually simple multiferroic in which the magnetic-field-driven flop of conical spin spirals leads to the simultaneous reversal of magnetization and electric polarization.

Highlights

  • Despite remarkable progress in developing multifunctional materials, spin-driven ferroelectrics featuring both spontaneous magnetization and electric polarization are still rare

  • We demonstrate experimentally that the effective spiral handedness, which is usually controlled by an electric field in magnetic spiral ferroelectrics, couples with P and with M via the C,Q domain switching, and its sign can be reversed by a magnetic field in Mn2GeO4

  • To prove the existence of the U coupling term (equation (1)), we studied the effect of a cooling electric field Ecool on spin-helicity in the Q domains using polarized neutron diffraction (spherical neutron polarimetry (SNP)) at TASP, Paul Scherrer Institut (PSI)

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Summary

Introduction

Despite remarkable progress in developing multifunctional materials, spin-driven ferroelectrics featuring both spontaneous magnetization and electric polarization are still rare. Among such ferromagnetic ferroelectrics are conical spin spiral magnets with a simultaneous reversal of magnetization and electric polarization that is still little understood Such materials can feature various multiferroic domains that complicates their study. One of the few systems exhibiting both spontaneous M and P is a spiral magnet with the so-called transverse conical spin structure, which consists of a cycloidal spiral spin component and a ferromagnetic component along the spin rotation axis of the cycloid[3,6] This is an example of a so-called multi-Q structure in which two distinct magnetic propagation vectors Q coexist. This structure is described by two irreps D1 and D2, and contains a cycloidal component which can be responsible for

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