Mathematical Model for Biomolecular Quantification Using Large-Area Surface-Enhanced Raman Spectroscopy Mapping.

Mathematical Model for Biomolecular Quantification Using Large-Area Surface-Enhanced Raman Spectroscopy Mapping.
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使用大面积表面增强拉曼光谱映射进行生物分子定量的数学模型。

DOI:
10.1039/c5ra16108h
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发表时间:
2015
期刊:
影响因子:
3.9
通讯作者:
Boisen,Anja
Boisen,Anja
中科院分区:
化学3区
文献类型:
--
作者:
Palla,Mirkó;Bosco,FilippoG;Yang,Jaeyoung;Rindzevicius,Tomas;Alstrom,TommyS;Schmidt,MichaelS;Lin,Qiao;Ju,Jingyue;Boisen,Anja

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基于纳米结构平台的表面增强拉曼光谱(SERS)是分析生物化学领域中一种极具前景的生物分子定量和高灵敏度检测技术。在这里,我们报告了一个数学模型来预测目标分子在受体功能化纳米柱底物上的实验SERS信号(或热点)强度分布,用于生物分子定量。我们证明,仅利用一小组经验确定的参数,我们的一般理论框架与实验数据在皮摩尔浓度制度下特别好地一致。该模型可广泛用于具有平面几何形状的SERS基底上的拉曼映射,其中热点近似为由紧密间隔的二聚体产生的电磁增强场。最后,我们还发现tamra标记的抗利尿激素特异性靶分子的检测限接近单分子水平,从而在SERS定量领域开辟了令人兴奋的新篇章。
Surface-enhanced Raman spectroscopy (SERS) based on nanostructured platforms is a promising technique for quantitative and highly sensitive detection of biomolecules in the field of analytical biochemistry. Here, we report a mathematical model to predict experimental SERS signal (or hotspot) intensity distributions of target molecules on receptor-functionalized nanopillar substrates for biomolecular quantification. We demonstrate that by utilizing only a small set of empirically determined parameters, our general theoretical framework agrees with the experimental data particularly well in the picomolar concentration regimes. This developed model may be generally used for biomolecular quantification using Raman mapping on SERS substrates with planar geometries, in which the hotspots are approximated as electromagnetic enhancement fields generated by closely spaced dimers. Lastly, we also show that the detection limit of a specific target molecule, TAMRA-labeled vasopressin, approaches the single molecule level, thus opening up an exciting new chapter in the field of SERS quantification.