Emergent $d$-wave altermagnetism in orthogonally twisted bilayer CrPS$_4$

Abstract

Twistronics is a powerful strategy to engineer novel quantum states by controlling the relative orientation between layered materials. Here, we demonstrate that an orthogonally twisted bilayer CrPS$_4$ shows $d$-wave altermagnetism driven purely by structural rotation. Symmetry analysis reveals that the twisted stacking breaks partial translational combined with time-reversal symmetry, leading to a fourfold rotation relation between opposite spin sublattices, enabling altermagnetism. First-principles calculations demonstrate a sizable non-relativistic spin splitting of up to 68 meV around the Fermi level. We further show that the altermagnetic state can be further stabilized through interlayer compression and modulation of the on-site Coulomb interaction. The resulting band structure exhibits pronounced spin-dependent anisotropy, enabling efficient spin to charge conversion reaching $\sim$50% near the Fermi level and sizable giant magnetoresistance. These results establish twisted CrPS$_4$ as a realistic platform for altermagnetism and highlights twistronics as a versatile route for advanced spintronics applications.