Core-Shell Perovskite Quantum Dots for Highly Selective Room-Temperature Spin Light-Emitting Diodes

Adv Mater. 2024 Feb;36(5):e2309335. doi: 10.1002/adma.202309335. Epub 2023 Dec 5.

Abstract

Circularly polarized light (CPL) is a crucial light source with a wide variety of potential applications such as magnetic recording, and 3D display. Here, core-shell heterostructured perovskite quantum dots (QDs) for room-temperature spin-polarized light-emitting diodes (spin-LEDs) are developed. Specifically, a 2D chiral perovskite shell is deposited onto the achiral 3D inorganic perovskite (CsPbBr3 ) core. Owing to the chiral-induced spin selectivity effect, the spin state of the injected charge carriers is biased when they are transmitted through the 2D chiral shell. The spin-controlled carriers then radiatively recombine inside the CsPbBr3 emissive core, resulting in CPL emission. It is demonstrated that the (R)- and (S)-1-(2-(naphthyl)ethylamine) (R-/S-NEA) 2D chiral cations enhance the spin polarization degree due to their strong chiroptical properties. Systematical defect analyses confirm that 2D chiral cations (i.e., R-/S-NEA) successfully passivate halide vacancies at the surface of the CsPbBr3 QDs, thereby attaining a high photoluminescence quantum yield of 78%. Moreover, the spin-LEDs prepared with core-shell QDs achieve a maximum external quantum efficiency of 5.47% and circularly polarized electroluminescence with a polarization degree (PCP-EL ) of 12% at room temperature. Finally, various patterns fabricated by inkjet printing the core-shell QDs emit strong CPL, highlighting their potential as an emitter for next-generation displays.

Keywords: chiral-induced spin selectivity; core-shell; nanocrystals; perovskite; spin-LEDs.