The effect of DNA bases permutation on surface-enhanced Raman scattering spectrum
The effect of DNA bases permutation on surface-enhanced Raman scattering spectrum
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DOI：
10.1515/nanoph-2021-0021
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发表时间：
2021-02
期刊：
影响因子：
7.5
通讯作者：
Shimon Rubin;Phuong H. L. Nguyen;Y. Fainman
中科院分区：
文献类型：
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作者：
Shimon Rubin;Phuong H. L. Nguyen;Y. Fainman
摘要表面增强拉曼散射（Sers）过程导致吸附在等离子体金属上的分子的拉曼散射截面显著增加，并受到金属表面几何结构、光学性质、化学吸附分子取向和化学环境等诸多物理化学因素的影响。虽然Sers有望用于DNA序列的单分子灵敏度和光学传感，但需要更详细地了解各种因素之间丰富的物理化学相互作用，以提高现有和未来基于SERS的DNA传感平台的预测能力。在这项工作中，我们报告的实验结果表明，吸附的单链DNA（ssDNA）异构体的Sers光谱依赖于单个碱基出现在3个碱基长的ssDNA由于DNA碱基之间的分子内相互作用的顺序。此外，我们的实验表明，该效果持有在更一般的条件下，当分子不经历化学增强，由于共振电荷转移效应，也在标准的拉曼散射没有电磁或化学增强。我们的数值模拟定性地支持了实验结果，并表明基置换的结果在修改的拉曼和化学增强拉曼光谱。
Abstract Surface-enhanced Raman scattering (SERS) process results in a tremendous increase of Raman scattering cross section of molecules adsorbed to plasmonic metals and influenced by numerous physico-chemical factors such as geometry and optical properties of the metal surface, orientation of chemisorbed molecules and chemical environment. While SERS holds promise for single molecule sensitivity and optical sensing of DNA sequences, more detailed understanding of the rich physico-chemical interplay between various factors is needed to enhance predictive power of existing and future SERS-based DNA sensing platforms. In this work, we report on experimental results indicating that SERS spectra of adsorbed single-stranded DNA (ssDNA) isomers depend on the order on which individual bases appear in the 3-base long ssDNA due to intramolecular interaction between DNA bases. Furthermore, we experimentally demonstrate that the effect holds under more general conditions when the molecules do not experience chemical enhancement due to resonant charge transfer effect and also under standard Raman scattering without electromagnetic or chemical enhancements. Our numerical simulations qualitatively support the experimental findings and indicate that base permutation results in modification of both Raman and chemically enhanced Raman spectra.