Design of Two-Dimensional Hybrid Perovskites with Giant Spin Splitting and Persistent Spin Textures

Semiconductors with large energetic separation Δ<i>E</i>^± of energy sub-bands with distinct spin expectation values (spin textures) represent a key target to enable control over spin transport and spin-optoelectronic properties. While the paradigmatic case of symmetry-dictated Rashba spin splitting and associated spin textures remains the most explored pathway toward designing future spin-transport-based quantum information technologies, controlling spin physics beyond the Rashba paradigm by accessing strategically targeted crystalline symmetries holds significant promise. In this paper, we show how breaking the traditional paradigm of octahedron-rotation based structure distortions in 2D organic-inorganic perovskites (2D-OIPs) can facilitate exceptionally large spin splittings (Δ<i>E</i>^± > 400 meV) and spin textures with extremely short spin helix lengths (<i>l</i>_PSH ∼ 5 nm). A simple bond angle difference captures the distortion-driven global asymmetry and correlates quantitatively with first-principles computed spin-splitting magnitudes. A multiband effective mass model that accounts for interlayer coupling provides a unified understanding of how specific symmetry elements dictate layer- and state-dependent spin polarizations within these multi-quantum-well structures. The general symmetry analysis methodology presented here, together with the potential for rationally creating 2D-OIPs with unique symmetry patterns, opens a pathway to design semiconductors with outstanding spin properties for next generation opto-spintronics.