Fig. 4: Spin-selective hot carrier relaxation of 2D Dion–Jacobson perovskites.

a Scheme for the optical selection for the circular polarized TA measurements of 2D DJ perovskite films. Right (left) circular polarized light σ+ (σ−) couples to the electronic transition from the valence bands to high-level conduction bands. Extracted hot-carrier temperature as a function of delay time of (b) (3AMP)PbI4 and (c) (4AMP)PbI4 obtained from cocircular (σ+σ+ and σ−σ−) and counter circular (σ+σ− and σ−σ+) polarized pump-probe TA spectra. d Time evolution of hot-electron relaxation starting from the two split bands for (3AMP)PbI4 calculated with consideration of spin-orbit coupling and decoherence effects. e Schematic illustration of the hot-electron relaxation processes in 2D DJ perovskites without and with band splitting and of the spin-flip/precession and scattering processes in (4AMP)PbI4.