Optimizing the Shelling Process of InP/ZnS Quantum Dots Using a Single-Source Shell Precursor: Implications for Lighting and Display Applications

This is the data supporting the manuscript "Optimizing the Shelling Process of InP/ZnS Quantum Dots Using a Single-Source Shell Precursor: Implications for Lighting and Display Applications". Abstract InP/ZnS core/shell quantum dots (QDs), recognized as highly promising heavy-metal-free emitters, are increasingly utilized in lighting and display applications. Their synthesis in a tubular flow reactor enables production in a highly efficient, scalable, and reproducible manner, particularly when combined with a single-source shell precursor, such as zinc diethyldithiocarbamate (Zn(S2CNEt2)2). However, the photoluminescence quantum yield (PLQY) of QDs synthesized with this route remains significantly lower compared to those synthesized in batch reactors involving multiple steps for the shell growth. Our study identifies the formation of absorbing, yet non-emissive ZnS nanoparticles during the ZnS shell formation process as a main contributing factor to this discrepancy. By varying the shelling conditions, especially the shelling reaction temperature and InP core concentration, we investigated the formation of pure ZnS nanoparticles and their impact on the optical properties, particularly PLQY, of the resultant InP/ZnS QDs through UV-vis absorption, steady-state and time-resolved photoluminescence (PL) spectroscopy, scanning transmission electron microscopy (STEM) and analytical ultracentrifugation (AUC) measurements. Our results suggest that process conditions, such as lower shelling temperatures or reduced InP core concentrations (resulting in a lower external surface area), encourage the homogeneous nucleation of ZnS. This reduces the availability of shell precursors necessary for an effective passivation of the InP core surfaces, ultimately resulting in lower PLQYs. These findings explain the origin of persistently underperformed PLQY of InP/ZnS QDs synthesized from this synthesis route and suggest further optimization strategies to improve their emission for lighting and display applications. The data are sorted per techniques used for characterization. Information about the measurement details can be found in README file.本数据集支撑题为《采用单源壳层前驱体优化InP/ZnS量子点壳层工艺：及其在照明与显示应用中的启示》的研究手稿。 摘要 InP/ZnS核壳量子点（InP/ZnS core/shell quantum dots, QDs）被公认为极具应用潜力的无重金属发光体，正日益广泛应用于照明与显示领域。通过管式流动反应器进行合成，可实现高效、可规模化且可重复的生产，尤其当结合单源壳层前驱体时，例如二乙基二硫代氨基甲酸锌（zinc diethyldithiocarbamate, Zn(S2CNEt2)2）。然而，采用该路线合成的量子点的光致发光量子产率（photoluminescence quantum yield, PLQY），仍显著低于采用多步骤壳层生长工艺的分批反应器合成的量子点。本研究发现，在ZnS壳层形成过程中产生的吸光但不发光的ZnS纳米颗粒，是造成这一性能差异的主要诱因。本研究通过调控壳层生长条件，尤其是壳层反应温度与InP核浓度，结合紫外-可见吸收光谱（UV-vis absorption）、稳态与时间分辨光致发光（steady-state and time-resolved photoluminescence, PL）光谱、扫描透射电子显微镜（scanning transmission electron microscopy, STEM）以及分析超速离心（analytical ultracentrifugation, AUC）表征手段，探究了纯ZnS纳米颗粒的形成过程，及其对所得InP/ZnS QDs光学性能（尤其是PLQY）的影响。研究结果表明，较低的壳层生长温度或降低的InP核浓度（导致更低的外比表面积）会促进ZnS的均相成核。这会减少有效钝化InP核表面所需的壳层前驱体用量，最终导致更低的PLQY。本研究结果阐释了采用该合成路线得到的InP/ZnS QDs的PLQY始终偏低的根源，并提出了进一步优化其发光性能的策略，以适配照明与显示应用。 本数据集按照表征所用的技术类别进行分类。测试细节可查阅README文件。