Managing Edge States in Reduced‐Dimensional Perovskites for Highly Efficient Deep‐Blue LEDs

Pure-halide reduced-dimensional perovskites, featuring large exciton binding energy and tunable bandgap, show great potential for high-efficiency deep-blue perovskite light-emitting diodes (PeLEDs). However, their efficiency, particularly in the low n-value phase domain ("n" represents the number of octahedral sheets), lags behind analogous perovskite emitters. Herein, it is demonstrated that the vibration of edge-dangling octahedra in the low n-value phase activates notorious exciton-phonon (EP) coupling, thereby deteriorating efficiency. To address this issue, an approach is reported to manage edge-state lattices by introducing tris(4-fluorophenyl) phosphine (TFP) ligands. Attributed to the large steric hindrance of TFP ligands and their strong binding affinity for edge-dangling octahedra, the edged-octahedral tilting reconstruction can effectively suppress lattice vibration and inhibit EP coupling. This strategy yields deep-blue emitting film with a spectral linewidth of 21 nm and a photoluminescence quantum yield of 85% at low excitation densities. The resulting PeLEDs achieve deep-blue emission at 469 nm, with a maximum luminance of 2,428 cd m^-2 and a maximum external quantum efficiency of 10.4%, marking them among the most efficient deep-blue PeLEDs reported. The strategy also showcases universality for higher n-value reduced-dimensional perovskites. It is believed that the observation, along with the edge-state management strategy, lays the groundwork for further advancements in reduced-dimensional perovskite optoelectronic devices.