Sun Zhenli, Du Jingjing, Yan Li, Chen Shu, Yang Zhilin, Jing Chuanyong
State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences , Beijing 100085, China.
Department of Physics, Xiamen University , Xiamen 361005, China.
ACS Appl Mater Interfaces. 2016 Feb 10;8(5):3056-62. doi: 10.1021/acsami.5b10230. Epub 2016 Jan 26.
Nanofabrication of multifunctional surface-enhanced Raman scattering (SERS) substrates is strongly desirable but currently remains a challenge. The motivation of this study was to design such a substrate, a versatile core-satellite Fe3O4@SiO2-Au (FA) hetero-nanostructure, and demonstrate its use for charge-selective detection of food dye molecules as an exemplary application. Our experimental results and three-dimensional finite difference time domain (FDTD) simulation suggest that tuning the Au nanoparticle (NP) gap to sub-10 nm, which could be readily accomplished, substantially enhanced the Raman signals. Further layer-by-layer deposition of a charged polyelectrolyte on this magnetic SERS substrate induced active adsorption and selective detection of food dye molecules of opposite charge on the substrates. Molecular dynamics (MD) simulations suggest that the selective SERS enhancement could be attributed to the high affinity and close contact (within a 20 Å range) between the substrate and molecules. Density function theory (DFT) calculations confirm the charge transfer from food dye molecules to Au NPs via the polyelectrolytes. This multifunctional SERS platform provides easy separation and selective detection of charged molecules from complex chemical mixtures.
多功能表面增强拉曼散射(SERS)基底的纳米制造非常必要,但目前仍是一项挑战。本研究的目的是设计这样一种基底,即一种通用的核壳型Fe3O4@SiO2-Au(FA)异质纳米结构,并展示其作为典型应用用于食品染料分子电荷选择性检测的用途。我们的实验结果和三维时域有限差分(FDTD)模拟表明,将金纳米颗粒(NP)间隙调整到10纳米以下(这很容易实现),可大幅增强拉曼信号。在这种磁性SERS基底上进一步逐层沉积带电聚电解质,可诱导基底对相反电荷的食品染料分子进行主动吸附和选择性检测。分子动力学(MD)模拟表明,选择性SERS增强可归因于基底与分子之间的高亲和力和紧密接触(在20 Å范围内)。密度泛函理论(DFT)计算证实了食品染料分子通过聚电解质向金纳米颗粒的电荷转移。这种多功能SERS平台可轻松从复杂化学混合物中分离和选择性检测带电分子。