Se/S Ratio-Dependent Properties and Application of Gradient-Alloyed CdSeS Quantum Dots: Shell-free Structure, Non-blinking Photoluminescence with Single-Exponential Decay, and Efficient QLEDs.

Colloidal quantum dots (QDs) are promising optical and optoelectronic materials for various applications. The excited state properties are important indexes to assess the quality of QDs and may directly affect their applications. Different from controlling surface engineering (surface ligands, shell thickness, etc.) to adjust excited state properties, high-quality shell-free alloyed CdSeS (simplified as CdSeS) QDs with controlled excited state properties were synthesized by tuning the composition and using diphenylphosphine as a beneficial additive at a low temperature (∼180 °C). The optimized CdSeS shell-free alloyed QDs (Se/S = 1:8) exhibited excellent optical properties with tuning of the excited state, including single-exponential photoluminescence (PL) decay dynamics, a narrow full width at half maximum of 28 nm, and non-blinking emission behavior (>98% "on" time). Furthermore, all-solution-processed, multilayered quantum dot light-emitting diodes were fabricated using the conventional device structure to assess the performance of QDs with composition-controlled excited states. The best device displayed a maximum luminance of 92,330 cd m, a current efficiency of 50.3 cd A, and an external quantum efficiency of 14.5%.