Tunable Rashba Spin Splitting in Two-Dimensional Polar Perovskites

Two-dimensional (2D) Rashba semiconductors with structure inversion asymmetry and a spin-orbit coupling (SOC) effect show promising applications in nanospintronics, such as spin field effect transistors (FETs). Here, we systematically investigate the electronic structures and Rashba effect of 2D polar perovskites ABX₃ (A = Cs⁺ or Rb⁺; B = Pb²⁺ or Sn²⁺; X = Cl, Br, or I) by first-principles density functional theory calculations. We demonstrate that, except for the cubic case, 2D polar perovskites from tetragonal and orthorhombic three-dimensional (3D) bulks exhibit a strong intrinsic Rashba effect around the Γ point, due to their structure inversion asymmetry and the strong SOC effect of heavy atoms. In particular, 2D orthorhombic RbSnI₃ shows the largest Rashba constant of 1.176 eV Å among these polar perovskites, which is comparable to that of 3D bulk perovskites previously reported in experiments and theory. Furthermore, several 2D polar perovskites also show a strong electric field response. In particular, 2D tetragonal RbPbI₃ and tetragonal CsPbI₃ have strong electric field responses of >0.5 e Ų. Therefore, 2D polar perovskites as promising Rashba semiconductors possess large Rashba constants and strong electric field responses, resulting in a short spin channel length of tens of nanometers to preserve the spin coherence in spin FETs, superior to conventional 3D micrometer spin FETs.