Improved Efficiency and Stability in Pure‐Red CdSe Nanoplatelet LEDs Enabled by Gradient Alloyed CdSeS/CdZnS Crown/Shell

Abstract Anisotropic nanoplatelets (NPLs) possess strong in‐plane transition dipole moments and out‐of‐plane emission, which enable a maximum photon out‐coupling efficiency of 40% and a high gain coefficient, making them ideal candidates for light‐emitting diodes (LEDs) and lasers. However, the unbalanced surface energy between the side and top facets of NPLs results in poor thermal stability and high susceptibility to ripening at elevated temperatures, which complicates the growth of the shell. To address this issue, a gradient crown (CdSeS) around the CdSe NPLs is designed to stabilize the high energy side facets. Consequently, the gradient alloyed shell (CdZnS) is successfully grown, and the CdSe/CdSeS/CdZnS core/crown/shell NPLs exhibited near‐unity photoluminescence quantum yield. The CdSeS/CdZnS crown/shell structure suppressed non‐radiative Auger recombinations, achieving a record‐low amplification spontaneous emission threshold of 2.11 µJ cm −2 under femtosecond laser excitation. In addition, by selecting the carrier transport layers with matched energy levels, the NPL‐LEDs demonstrate a record‐high external quantum efficiency of 30.1% in the pure‐red range, driven by the 94% in‐plane transition dipole moment distribution of NPL film. The NPL‐LEDs also exhibited a long operational lifetime of T 95 > 600 h at a luminance of 1000 cd m −2 .