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来自液体前驱体的胶体二维层状碳化硅量子点:表面钝化、明亮的光致发光和平面自组装

Colloidal 2D Layered SiC Quantum Dots from a Liquid Precursor: Surface Passivation, Bright Photoluminescence, and Planar Self-Assembly.

作者信息

Thomas Salim A, Alharthi Naif S, Petersen Reed J, Aldrees Ahmed, Tani Sakurako, Anderson Kenneth J, Granlie Joseph, Pringle Todd A, Payne Scott A, Choi Yongki, Kilin Dmitri S, Hobbie Erik K

机构信息

Materials & Nanotechnology Program, North Dakota State University, Fargo, North Dakota 58108, United States.

Department of Physics, North Dakota State University, Fargo, North Dakota 58108, United States.

出版信息

ACS Nano. 2024 Oct 1;18(39):26848-26857. doi: 10.1021/acsnano.4c08052. Epub 2024 Sep 17.

Abstract

We report the bottom-up synthesis of colloidal two-dimensional (2D) layered silicon carbide (SiC) quantum dots with a cubic structure, lateral size of 5-10 nm, ⟨110⟩ exfoliation to few atomic layers, and surface passivation with 1-dodecene. Samples shielded from oxygen and plasma-annealed for purity exhibit narrow blue photoluminescence (PL) with quantum yields (QYs) over 60% in exceptional cases, while unshielded nanocrystals (NCs) exhibit broad blue/green/white PL with 10-15% QY. The latter scenario is attributed to excess surface carbon and oxygen accrued during synthesis and processing, with size separation through ultracentrifugation revealing size-dependent impurity emission. In contrast, the shape of the bright narrow blue PL shows little variation with NC size, while in both scenarios, the maximum QY occurs near four atomic layers. When dried under heat, the disk-like NC suspensions are observed to aggregate into microscale domains, with further self-assembly into planar superlattice domains with common crystalline orientation. The results are compared with photophysical simulations and bring clarity to the broad emission commonly reported for top-down approaches, while inspiring bottom-up schemes directed at improved material quality.

摘要

我们报道了通过自下而上的方法合成具有立方结构、横向尺寸为5-10纳米、沿⟨110⟩方向剥离至几个原子层且用1-十二碳烯进行表面钝化的胶体二维(2D)层状碳化硅(SiC)量子点。对避免氧气影响并进行等离子体退火以提高纯度的样品而言,在特殊情况下会表现出窄的蓝色光致发光(PL),量子产率(QYs)超过60%,而未加保护的纳米晶体(NCs)则表现出宽的蓝色/绿色/白色PL,量子产率为10-15%。后一种情况归因于在合成和加工过程中积累的过量表面碳和氧,通过超速离心进行尺寸分离揭示了与尺寸相关的杂质发射。相比之下,明亮的窄蓝色PL的形状随纳米晶体尺寸变化不大,而在这两种情况下,最大量子产率出现在接近四个原子层处。当在加热条件下干燥时,观察到盘状纳米晶体悬浮液聚集成微米级区域,并进一步自组装成具有共同晶体取向的平面超晶格区域。将结果与光物理模拟进行了比较,为自上而下方法中普遍报道的宽发射现象提供了清晰解释,同时也为旨在提高材料质量的自下而上方案提供了启发。

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