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钙钛矿芯片上的单原子位点实现表面增强拉曼光谱的创纪录高灵敏度和定量分析。

Single-atom sites on perovskite chips for record-high sensitivity and quantification in SERS.

作者信息

Feng Ran, Miao Qing, Zhang Xiang, Cui Peixin, Wang Cong, Feng Yibo, Gan Liyong, Fu Jiaxing, Wang Shibo, Dai Ziyi, Hu Liming, Luo Yunjing, Sun Weihai, Zhang Xiaoxian, Xiao Jiawen, Wu Jinbo, Zhou Bingpu, Zou Mingqiang, He Dawei, Zhou Xiaoyuan, Han Xiaodong

机构信息

Beijing Key Laboratory of Microstructure and Properties of Solids, Institute of Microstructure and Property of Advanced Materials, Faculty of Materials and Manufacturing, Beijing University of Technology, Beijing, 100124 China.

Key Laboratory of Luminescence and Optical Information, Ministry of Education, Institute of Optoelectronic Technology, Beijing Jiaotong University, Beijing, 100044 China.

出版信息

Sci China Mater. 2022;65(6):1601-1614. doi: 10.1007/s40843-022-1968-5. Epub 2022 Mar 2.

Abstract

UNLABELLED

Surface enhanced Raman scattering (SERS) is a rapid and nondestructive technique that is capable of detecting and identifying chemical or biological compounds. Sensitive SERS quantification is vital for practical applications, particularly for portable detection of biomolecules such as amino acids and nucleotides. However, few approaches can achieve sensitive and quantitative Raman detection of these most fundamental components in biology. Herein, a noble-metal-free single-atom site on a chip strategy was applied to modify single tungsten atom oxide on a lead halide perovskite, which provides sensitive SERS quantification for various analytes, including rhodamine, tyrosine and cytosine. The single-atom site on a chip can enable quantitative linear SERS responses of rhodamine (10-1 mmol L), tyrosine (0.06-1 mmol L) and cytosine (0.2-45 mmol L), respectively, which all achieve record-high enhancement factors among plasmonic-free semiconductors. The experimental test and theoretical simulation both reveal that the enhanced mechanism can be ascribed to the controllable single-atom site, which can not only trap photoinduced electrons from the perovskite substrate but also enhance the highly efficient and quantitative charge transfer to analytes. Furthermore, the label-free strategy of single-atom sites on a chip can be applied in a portable Raman platform to obtain a sensitivity similar to that on a benchtop instrument, which can be readily extended to various biomolecules for low-cost, widely demanded and more precise point-of-care testing or detection.

ELECTRONIC SUPPLEMENTARY MATERIAL

Supplementary material is available for this article at 10.1007/s40843-022-1968-5 and is accessible for authorized users.

摘要

未标注

表面增强拉曼散射(SERS)是一种快速且无损的技术,能够检测和识别化学或生物化合物。灵敏的SERS定量对于实际应用至关重要,特别是对于便携式检测生物分子,如氨基酸和核苷酸。然而,很少有方法能够实现对生物学中这些最基本成分的灵敏且定量的拉曼检测。在此,一种芯片上无贵金属单原子位点策略被应用于修饰卤化铅钙钛矿上的单钨原子氧化物,这为包括罗丹明、酪氨酸和胞嘧啶在内的各种分析物提供了灵敏的SERS定量。芯片上的单原子位点能够分别实现罗丹明(10⁻¹ mmol/L)、酪氨酸(0.06 - 1 mmol/L)和胞嘧啶(0.2 - 45 mmol/L)的定量线性SERS响应,这些在无等离子体半导体中均实现了创纪录的高增强因子。实验测试和理论模拟均表明,增强机制可归因于可控的单原子位点,其不仅可以捕获来自钙钛矿基底的光生电子,还能增强向分析物的高效且定量的电荷转移。此外,芯片上单原子位点的无标记策略可应用于便携式拉曼平台,以获得与台式仪器相似的灵敏度,这可以很容易地扩展到各种生物分子,用于低成本、广泛需求且更精确的即时检测或诊断。

电子补充材料

本文的补充材料可在10.1007/s40843 - 022 - 1968 - 5获取,授权用户可访问。

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