Abstract

Entanglement of the spin–orbit and magnetic order in multiferroic materials bears a strong potential for engineering novel electronic and spintronic devices. Here, we explore the electron and spin structure of ferroelectric α-GeTe thin films doped with ferromagnetic Mn impurities to achieve its multiferroic functionality. We use bulk-sensitive soft-X-ray angle-resolved photoemission spectroscopy (SX-ARPES) to follow hybridization of the GeTe valence band with the Mn dopants. We observe a gradual opening of the Zeeman gap in the bulk Rashba bands around the Dirac point with increase of the Mn concentration, indicative of the ferromagnetic order, at persistent Rashba splitting. Furthermore, subtle details regarding the spin–orbit and magnetic order entanglement are deduced from spin-resolved ARPES measurements. We identify antiparallel orientation of the ferroelectric and ferromagnetic polarization, and altering of the Rashba-type spin helicity by magnetic switching. Our experimental results are supported by first-principles calculations of the electron and spin structure.

Highlights

  • Entanglement of the spin–orbit and magnetic order in multiferroic materials bears a strong potential for engineering novel electronic and spintronic devices

  • We show that multiferroic Ge1 À xMnxTe inherits from its parent FE a-GeTe compound a giant Rashba splitting of threedimensional (3D) bulk states[12,13,14], which competes with the Zeeman spin splitting induced by the magnetic exchange interactions

  • We use SX-ARPES to elucidate the local electronic structure of the Mn ions and RZ splitting with 3D k-space resolution, and spinresolved ARPES (SARPES) in the ultraviolet photon energy range to explore the corresponding changes in the spin textures in this multiferroic material

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Summary

Introduction

Entanglement of the spin–orbit and magnetic order in multiferroic materials bears a strong potential for engineering novel electronic and spintronic devices. Superconductors with sizable Rashba spin splitting and ferromagnetic (FM) order would unite all ingredients for formation and manipulation of so-called anyons, generalizing the concept of Majorana fermions[7] The collinear alignment of FE and FM polarization leads to an opening of a tunable Zeeman gap of up to 100 meV around the Dirac point of the Rashba bands, coupled with a change in spin texture by entanglement of magnetic and spin–orbit order. Considering the momentum-dependent expected values of the spin components in all directions, only systems with magnetization parallel to the inversion symmetry breaking direction can reorient the spin of the Rashba electrons and open a gap in all k|| directions as illustrated by Fig. 1g and Supplementary Fig. 1 (Supplementary Note 1.1).

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