Multistate control in 2D CuCrP2S6/Sc2CO2 multiferroic heterostructures

Abstract

The magnetoelectric (ME) coupling effect enables effective cross-control between electric and magnetic fields, providing a crucial pathway toward next-generation low-power electronic devices. Here, we propose a two-dimensional (2D) multistate multiferroic heterostructure (MMH) composed of out-of-plane polarized CuCrP2S6 and Sc2CO2 (CCPS/SCO) to realize electric field driven multistate spintronic devices. First-principles calculations demonstrate that the CCPS/SCO heterostructure can be reversibly switched among four nonvolatile polarization states (↑↑, ↑↓, ↓↓, ↓↑) using electrical pulses, enabling simultaneous control of electronic transport, magnetic ordering, and spin orientation within a single heterostructure. By encoding the four polarization states, three distinct quantum phases are identified, i.e., out-of-plane antiferromagnetic metal, in-plane ferromagnetic semiconductor, and out-of-plane ferromagnetic metal. The microscopic mechanism underlying this strong ME coupling originates from polarization-induced interfacial charge transfer and symmetry breaking, which synergistically shift the energy level and tune the orbital occupation of Cr-d orbitals. Our proposed CCPS/SCO MMH heterostructure establishes a promising platform for high-density, low-power, and functionally reconfigurable spintronic memory.