Joo Sung Kim, Hyeon‐Dong Lee, Jeong Hyun Jung, Taehee Kim, Seung‐Je Woo, Hyung Joong Yoon, Jaehyun Moon, Chan‐mo Kang, S. Chang, Dong‐Hyeok Kim, Sungjin Kim, Sungjin Kim, Hoichang Yang, Dongho Kim, Dongho Kim, Tae‐Woo Lee
Abstract Quasi-two-dimensional perovskite structures hold great potential as active layers in blue perovskite light-emitting diodes. However, they face challenges of limited emission efficiency and broadened spectra due to phase inhomogeneity. Here, we report an intermediate-direct-pinning method to develop a uniform-phase quasi-two-dimensional structure with a homogeneous energy landscape. By forming a strong cation-π interaction complex, we stabilize a metastable intermediate phase with retarded crystallization toward low- n phases ( n ≤ 3), followed by a direct pinning process favouring crystallization of medium- n phases ( n = 4 and 5) without further broadening. Additionally, introducing a surface-anchoring ligand during the pinning process effectively suppresses non-radiative recombination. The resultant structure shows efficient sky-blue emission and narrow linewidth (108 meV). Devices fabricated with this structure reach a maximum external quantum efficiency of 22.5% at 489 nm, which is scalable to large-area (pixel size: 900 mm 2 ) and passive matrix devices (30 × 10 arrays, active area = 200 μm × 600 μm). These findings highlight the potential of perovskite light-emitting diodes for full-colour displays.