Designing Spin-driven Multiferroics in Altermagnets

Abstract: Spin-driven multiferroics exhibit strong magnetoelectric coupling, with notable polarization changes under a magnetic field, but these effects are usually limited to high-Z magnetic insulators with low electronic polarization. In this work, we introduce altermagnets as a promising platform for achieving strong magnetoelectric coupling in low-Z systems with substantial polarization. This large polarization arises from a design principle that utilizes the Heisenberg-like exchange striction mechanism, eliminating the reliance on spin-orbit coupling (SOC). This approach enables the Kramers-degenerate antiferromagnetic phase derived from altermagnetic insulators to achieve substantial polarization without spin splitting, providing a flexible platform for regulating spin-splitting phenomena. Through first-principles simulations and an effective Landau-Ginzburg Hamiltonian, we demonstrate that materials in the LiMnO2 family and strained RuF4 family can achieve polarization values exceeding 1.0 {\mu}C/cm2, an order of magnitude larger than those found in SOC-driven multiferroics. Moreover, their magnetoelectric coupling is one to two orders of magnitude stronger than that observed in conventional multiferroics and those driven by SOC.