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梯度带隙工程化合金化四元/三元CdZnSeS/ZnSeS量子点:共轭分子信标系统中用于流感病毒RNA生物传感的超灵敏荧光报告分子。

Gradient band gap engineered alloyed quaternary/ternary CdZnSeS/ZnSeS quantum dots: an ultrasensitive fluorescence reporter in a conjugated molecular beacon system for the biosensing of influenza virus RNA.

作者信息

Adegoke Oluwasesan, Seo Min-Woong, Kato Tatsuya, Kawahito Shoji, Park Enoch Y

机构信息

Laboratory of Biotechnology, Research Institute of Green Science and Technology, Shizuoka University, 836 Ohya, Suruga-ku, Shizuoka 422-8529, Japan.

出版信息

J Mater Chem B. 2016 Feb 28;4(8):1489-1498. doi: 10.1039/c5tb02449h. Epub 2016 Feb 4.

DOI:10.1039/c5tb02449h
PMID:32263115
Abstract

Controlling and engineering the particle composition of semiconductor alloys is one of the topmost targets in the field of semiconductor materials science and technology. Quantum dot (QD) nanocrystals offer an unmatched opportunity to obtain a wide range of composition-controlled alloys and have captivated a great deal of interest recently. Herein, we report on band gap engineering via tuning and controlling the sulphur molar fraction (ternary shell layer) of quaternary/ternary core/shell alloyed CdZnSeS/ZnSeS QDs. Varying optical properties were exhibited by the alloyed QDs but a uniform particle size distribution was maintained across all the compositions. The alloyed QDs displayed bright emission colours under UV irradiation, whereas the photoluminescence quantum yields (PL QY) were in a remarkable range of 36-98%. Non-linearity of the lattice parameter was an indication of gradient alloying of the nanocrystals, whereas the kinetics of the optical properties unravelled the effect of intrinsic optical bowing. Displacement of bond length and anion mismatch influenced the optical properties of the QDs with respect to the variation in the PL QY. Alloyed CdZnSeS/ZnSeS QDs with a spectacular PL QY were exploited as an ultrasensitive fluorescence reporter in a conjugated molecular beacon (MB) assay to detect influenza virus H1N1 RNA. Our detection system was rapid and highly sensitive for detecting extremely low concentrations of H1N1 RNA (down to 2 copies per mL), specific and versatile (detects H1N1 RNA in human serum). For proof of concept, the alloyed CdZnSeS/ZnSeS QD-MB bioprobe exhibited a superior 12-fold sensitivity over an alloyed CdZnSeS-MB probe, while a conventional CdSe/ZnS-MB probe could not detect extremely low concentrations of influenza virus H1N1 RNA.

摘要

控制和调控半导体合金的颗粒组成是半导体材料科学与技术领域的首要目标之一。量子点(QD)纳米晶体为获得各种成分可控的合金提供了无与伦比的契机,并且最近引起了广泛关注。在此,我们报道了通过调节和控制四元/三元核/壳合金化的CdZnSeS/ZnSeS量子点的硫摩尔分数(三元壳层)来进行带隙工程。合金化量子点展现出不同的光学性质,但在所有成分中均保持了均匀的粒径分布。合金化量子点在紫外线照射下呈现出明亮的发射颜色,而光致发光量子产率(PL QY)在36%至98%的显著范围内。晶格参数的非线性表明了纳米晶体的梯度合金化,而光学性质的动力学揭示了本征光学弯曲的影响。键长的位移和阴离子失配影响了量子点相对于PL QY变化的光学性质。具有出色PL QY的合金化CdZnSeS/ZnSeS量子点被用作共轭分子信标(MB)分析中的超灵敏荧光报告物,以检测甲型H1N1流感病毒RNA。我们的检测系统对于检测极低浓度的H1N1 RNA(低至每毫升2个拷贝)快速且高度灵敏,具有特异性和通用性(可检测人血清中的H1N1 RNA)。为了验证概念,合金化的CdZnSeS/ZnSeS量子点 - MB生物探针相对于合金化的CdZnSeS - MB探针表现出高达12倍的卓越灵敏度,而传统的CdSe/ZnS - MB探针无法检测极低浓度的甲型H1N1流感病毒RNA。

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