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Halide-Assisted Synthesis of Cadmium Chalcogenide Nanoplatelets

机译:卤化物辅助合成硫族化镉纳米片

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Atomically flat colloidal semiconductor CdSe nanoplatelets (NPLs) with precisely controlled thickness possess a range of unique optoelectronic properties. Here, we study the growth of CdSe, CdTe, and CdS NPLs with the aim of synthesizing thicker NPLs in order to extend their optical activity further into the lower energy/larger wavelength range. We employ cadmium halides, which lead to faster reaction kinetics as confirmed by control experiments with cadmium hydroxide as a Cd-precursor. Addition of halides in all cases led to the formation of thicker NPL species, as compared with the corresponding syntheses without these additives. Analysis of a recent theoretical model of the platelet growth mechanism confirms an earlier suggestion that reducing both the reaction enthalpy and the surface energy of CdSe, by replacing acetate ligands with chloride ions, should indeed lead to thicker NPLs as observed. We noticed a formation of Cd-0-metal nanoparticles in the first stage of the synthesis by preparing the Cd-precursor, which is another key finding of our work. We assume that these particles can serve as an active cadmium source facilitating the growth of the NPLs. The resulting 6 ML CdSe NPLs exhibited bright photoluminescence with quantum yield of up to 50, exceptionally narrow spectrum centered at 582 nm with full width at half-maximum of approx. 11 nm, and small Stokes shift of 2 nm. Moreover, we demonstrated the synthesis of heterostructured core/shell CdSe/CdS NPLs based on 6 ML CdSe platelets, which also exhibited bright fluorescence. This work shows the possibility to overcome energetic barrier limiting the size (thickness) control by using appropriate promoters of the growth of CdSe, CdTe, and CdS 2D structures.
机译:原子扁平胶体半导体CdSe纳米片(NPL)具有精确控制的厚度,具有一系列独特的光电特性。在这里,我们研究了 CdSe、CdTe 和 CdS NPL 的生长,目的是合成更厚的 NPL,以便将其光学活性进一步扩展到较低能量/更大的波长范围。我们采用卤化镉,这导致了更快的反应动力学,正如以氢氧化镉作为镉前体的对照实验所证实的那样。与没有这些添加剂的相应合成相比,在所有情况下添加卤化物都会导致形成更厚的NPL物质。对最近血小板生长机制理论模型的分析证实了一个早期的建议,即通过用氯离子取代乙酸盐配体来降低CdSe的反应焓和表面能,确实应该导致更厚的NPL。我们注意到在合成的第一阶段,通过制备Cd前驱体,形成了Cd-0金属纳米颗粒,这是我们工作的另一个关键发现。我们假设这些颗粒可以作为活性镉源,促进不良贷款的生长。所得的6 ML CdSe NPL表现出明亮的光致发光,量子产率高达50%,以582 nm为中心的超窄光谱,半峰处的全宽约为11 nm,小斯托克斯位移为2 nm。此外,我们展示了基于6 ML CdSe血小板的异质结构核壳CdSe/CdS NPLs的合成,该血小板也表现出明亮的荧光。这项工作表明,通过使用适当的 CdSe、CdTe 和 CdS 2D 结构生长促进剂来克服限制尺寸(厚度)控制的能量势垒的可能性。

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