Extremely Long Spin Lifetime of Light-Emitting States in Quasi-2D Perovskites through Orbit–Orbit Interaction

This paper reports an extremely long spin relaxation time of optically polarized light-emitting states at room temperature in quasi-2D perovskites [(PEA)2(MA)4Pb5Br16 with n = 5], when the long-range orbit–orbit interaction between excited states is developed through orbital polarization. Our studies found that the quasi-2D perovskite [(PEA)2(MA)4Pb5Br16 with n = 5] demonstrates a long-range orbit–orbit interaction between excited states to conserve the spins of optically polarized light-emitting states, identified by the positive change on photoluminescence intensity (+ΔPL) in steady state upon switching the photoexcitation from linear to circular polarization. Meanwhile, the PL circular polarization (σ+σ+ – σ+σ–) can maintain in nanosecond under fixed photoexcitation (σ+). In contrast, the 2D/3D mixed perovskite (n > 5) shows a short-range orbit–orbit interaction between excited states through orbital magnetic dipoles, identified by the −ΔPL by switching from linear to circular photoexcitation. At the same time, the spin lifetime of light-emitting states becomes undetectable.