Quantification of Chirality Induced Spin–Orbit Coupling for Long Spin Polarized Lifetime in Hybrid Perovskite

Long spin lifetimes are crucial for maintaining robust spin states during propagation in spintronic devices. Spin–orbit coupling (SOC) in chiral hybrid perovskites can induce chirality-dependent spin splitting, facilitating the manipulation of spin polarization. In this study, we introduce a chiral organic molecule, (<i>R</i>/<i>S</i>)-4-(aminoethyl)piperidinium (4AEP), into iodide-lead-based structures to synthesize chiral [(<i>R</i>/<i>S</i>)-4AEP]PbI₄ crystals and thin films. Using circularly polarized pump–probe techniques, we examine the carrier spin dynamics in [(<i>R</i>/<i>S</i>)-4AEP]PbI₄. Our results demonstrate that chirality-induced spin splitting significantly enhances the spin-polarization lifetime, achieving a spin splitting of approximately 130 meV at the valence band maximum and spin lifetimes exceeding 1 ns. Density functional theory (DFT) calculations reveal that opposite spin states exist in the <i>R</i>- and <i>S</i>-chiral samples with substantial spin splitting. These findings highlight the potential of chiral hybrid perovskites for spintronics applications.