Circularly polarized electroluminescence from thermally evaporated core-shell perovskite-based light-emitting diodes

Spin light-emitting diodes (spin-LEDs) have garnered significant attention for their potential applications in quantum information technology, three-dimensional displays, and secure optical communications. Although solution-processed spin-LEDs have advanced rapidly, they exhibit limited scalability and reproducibility. By contrast, spin-LEDs fabricated via thermal evaporation offer scalability and reproducibility but remain underdeveloped owing to uncontrolled crystallization and significant nonradiative recombination. In this study, we developed efficient perovskite spin-LEDs via multisource sequential evaporation utilizing PbBr 2 , chiral [1,1′-binaphthalene]-2,2′-diylbis[1,1-diphenyl-1,1′-phosphineoxide] (BINAPO) molecules, and CsBr. The chiral BINAPO molecules with bidentate (P = O) 2 groups surround the CsPbBr 3 lattice to form a perovskite–BINAPO structure. This structure controls perovskite crystallization, passivates surface defects, and enhances the exciton binding energy. Furthermore, the chiral-induced spin-selectivity effect of the chiral BINAPO shell alters the spin states of the injected carriers, which are subsequently transferred to the perovskite core, leading to the emergence of chiro-optical properties in the perovskite. The resulting perovskite spin-LEDs achieve maximum external quantum efficiencies of 13.20% (R-target) and 12.35% (S-target), in conjunction with electroluminescence dissymmetry factors of −0.124 (R-target) and 0.106 (S-target). This study presents the first demonstration of circularly polarized electroluminescence from thermally evaporated perovskite spin-LEDs, building a scalable platform for high-efficiency spin optoelectronics and practical perovskite spin-LEDs integration. This study presents a scalable strategy for circularly polarized perovskite light-emitting diodes (CP-PeLEDs) based on multisource sequential thermal evaporation, revealing how chiral molecular incorporation controls perovskite crystallization, spin-selective carrier dynamics, and chiro-optical emission. Precise crystal growth modulation using chiral BINAPO molecules forms an optimized perovskite–organic core–shell structure that suppresses nonradiative recombination and enhances exciton binding energy, while chiral-induced spin selectivity enables efficient spin transfer into the perovskite emissive core. This approach simultaneously improves device efficiency and circular polarization, providing a scalable pathway for high-performance perovskite spin optoelectronics and CP-PeLED integration. • First CP-EL from thermally evaporated perovskite spin-LEDs. • Bidentate (P = O)₂ in BINAPO coordinate with Pb²⁺ to enhance optoelectronic properties. • BINAPO shell serves as a CISS-active layer for spin control of injected carriers. • Spin-LED reached high EQE (13.2%) and g EL (0.124) at room temperature.