Origin of Rashba Spin-Orbit Coupling in 2D and 3D Lead Iodide Perovskites

We studied spin dynamics of charge carriers in the superlattice-like Ruddlesden-Popper hybrid lead iodide perovskite semiconductors, 2D (BA)(2)(MA)Pb(2)I(7) (with MA = CH(3)NH(3), and BA = CH(3)(CH(2))(3)NH(3)), and 3D MAPbI(3) using the magnetic field effect (MFE) on conductivity and electroluminescence in their light emitting diodes (LEDs) at cryogenic temperatures. The semiconductors with distinct structural/bulk inversion symmetry breaking, when combined with colossal intrinsic spin–orbit coupling (SOC), theoretically give rise to giant Rashba-type SOC. We found that the magneto-conductance (MC) magnitude increases monotonically with the emission intensity and saturates at ≈0.05% and 0.11% for the MAPbI(3) and (BA)(2)(MA)Pb(2)I(7), respectively. The magneto-electroluminescence (MEL) response with similar line shapes as the MC response has a significantly larger magnitude, and essentially stays constant at ≈0.22% and ≈0.20% for MAPbI(3) and (BA)(2)(MA)Pb(2)I(7), respectively. The sign and magnitude of the MC and MEL responses can be quantitatively explained in the framework of the Δg-based excitonic model using rate equations. Remarkably, the width of the MEL response in those materials linearly increases with increasing the applied electric field, where the Rashba coefficient in (BA)(2)(MA)Pb(2)I(7) is estimated to be about 7 times larger than that in MAPbI(3). Our studies might have significant impact on future development of electrically-controlled spin logic devices via Rashba-like effects.