Highly Emissive Lanthanide‐Based 0D Metal Halide Nanocrystals for Efficient Ultraviolet Photodetector

Abstract Recently, lanthanide‐based 0D metal halides have attracted considerable attention for their applications in X‐ray imaging, light‐emitting diodes (LEDs), sensors, and photodetectors. Herein, lead‐free 0D gadolinium‐alloyed cesium cerium chloride (Gd 3+ ‐alloyed Cs 3 CeCl 6 ) nanocrystals (NCs) are introduced as promising materials for optoelectronic application owing to their unique optical properties. The incorporation of Gd 3+ in Cs 3 CeCl 6 (CCC) NCs is proposed to increase the photoluminescence quantum yield (PLQY) from 57% to 96%, along with significantly enhanced phase and chemical stability. The structural analysis is performed by density functional theory (DFT) to confirm the effect of Gd 3+ in Cs 3 Ce 1‐ x Gd x Cl 6 (CCGC) alloy system. Moreover, the CCGC NCs are applied as the active layer in UVPDs with different Gd 3+ concentration. The excellent device performance is shown at 20% of Gd 3+ in CCGC NCs with high detectivity (7.938 × 10 11 Jones) and responsivity (0.195 A W −1 ) at ‐0.1 V at 310 nm. This study paves the way for the development of lanthanide‐based metal halide NCs for next‐generation UVPDs and other optoelectronic applications.