等离子体校准的无标记表面增强拉曼光谱仪，用于在癌症分型和药物测试中改善活细胞的多元分析,Analytical Chemistry

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等离子体校准的无标记表面增强拉曼光谱仪，用于在癌症分型和药物测试中改善活细胞的多元分析
Analytical Chemistry ( IF 6.7 ) Pub Date : 2021-03-05 , DOI: 10.1021/acs.analchem.0c05206
Wonil Nam ₁ , Xiang Ren ₁ , Inyoung Kim ₂ , Jeannine Strobl ₁ , Masoud Agah ₁ , Wei Zhou ₁

Affiliation

启用等离子纳米结构的无标记表面增强拉曼光谱仪（SERS）作为一种用于复杂生物样品的快速无损分子指纹表征技术，应运而生。但是，由于SERS信号对等离子体热点处局部光场变化的高度敏感性，无标签SERS生物分析面临着可靠性和可重复性方面的挑战，这可能会使所测量的光谱特征与复杂生化基质的实际分子浓度分布之间的相关性产生偏差。在本文中，我们报道了来自金属纳米结构的等离激元增强电子拉曼散射（ERS）信号可以用作SERS校准内标，以改善对生命生物系统的多变量分析。通过与未校准的SERS数据集进行并排比较，我们证明基于ERS的SERS校准可以增强（1）不同类型恶性程度的乳腺癌细胞亚型和（2）评估不同剂量下癌细胞的药物反应的无标记活细胞SERS光谱的监督学习分类。值得注意的是，基于ERS的SERS校准具有以下优势：在激光激发下具有出色的光稳定性，不会对生物分子拉曼信号产生光谱干扰，并且不会与热点处的生物分子竞争。因此，我们设想基于ERS的SERS校准可以显着提高活体生物系统和其他复杂生化矩阵的无标记SERS测量中的多元分析性能。

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Plasmonically Calibrated Label-Free Surface-Enhanced Raman Spectroscopy for Improved Multivariate Analysis of Living Cells in Cancer Subtyping and Drug Testing

Plasmonic nanostructure-enabled label-free surface-enhanced Raman spectroscopy (SERS) emerges as a rapid nondestructive molecular fingerprint characterization technique for complex biological samples. However, label-free SERS bioanalysis faces challenges in reliability and reproducibility due to SERS signals’ high susceptibility to local optical field variations at plasmonic hotspots, which can bias correlations between the measured spectroscopic features and the actual molecular concentration profiles of complex biochemical matrices. Herein, we report that plasmonically enhanced electronic Raman scattering (ERS) signals from metal nanostructures can serve as a SERS calibration internal standard to improve multivariate analysis of living biological systems. Through side-by-side comparisons with noncalibrated SERS datasets, we demonstrate that the ERS-based SERS calibration can enhance supervised learning classification of label-free living cell SERS spectra in (1) subtyping breast cancer cells with different degrees of malignancy and (2) assessing cancer cells’ drug responses at different dosages. Notably, the ERS-based SERS calibration has the advantages of excellent photostability under laser excitation, no spectral interference with biomolecule Raman signatures, and no occupation competition with biomolecules at hotspots. Therefore, we envision that the ERS-based SERS calibration can significantly boost the multivariate analysis performance in label-free SERS measurements of living biological systems and other complex biochemical matrices.

更新日期：2021-03-16

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