Understanding the Size‐Dependent Photostability and Photoluminescence Intermittency of Blue‐Emitting Core/Graded Alloy/Shell “giant”‐Quantum Dots

Abstract

Recently, giant quantum dots (g‐QDs) with a core/interface graded alloy shell/shell structure have shown promise in reducing photoluminescence (PL) intermittency and improving photostability. However, this approach has been mainly demonstrated with red and green emitting g‐QDs but the blue‐emitting graded alloy QDs has remained less explored. To tackle this challenge, a composition gradient method is employed to create three blue‐emitting CdZnS/CdxZn1–xS/ZnS core/interface graded alloy shell/shell (C/A/S) quantum dots (QDs) with different diameters. The sample with the largest diameter (gQD‐3) exhibits superior optical characteristics, with a photoluminescence quantum yield (PLQY) of approximately 62% and around 80% ON/radiative events at the single‐particle level. Conversely, the smallest diameter (gQD‐1) sample shows lower PLQY and only 30% radiative events with longer OFF/nonradiative events. Probability distribution analysis of PL trajectories, fitted with a truncated power law, reveals a significantly higher carrier de‐trapping rate in gQD‐3 compared to gQD‐1, attributed to its proximity to band edge trap states. Additionally, the largest diameter sample retains remarkable optical performance during 48 h of continuous UV irradiation in colloidal suspension and single‐particle levels. These findings show optimized core/shell structures, gradual alloy interfaces, and outer shell coatings can stabilize blue‐emitting quantum dots, advancing next‐gen optoelectronics.