Schorr Hannah C, Schultz Zachary D
Department of Chemistry and Biochemistry, The Ohio State University, Columbus, OH 43210, USA.
Analyst. 2024 Jul 8;149(14):3711-3715. doi: 10.1039/d4an00801d.
Surface enhanced Raman scattering (SERS) provides a label free method of analyzing molecules from diverse and complex signals, potentially with single molecule sensitivity. The chemical specificity inherent in the SERS spectrum can identify molecules; however signal variability arising from the diversity of plasmonic environments can limit quantification, particularly at low concentrations. Here we show that digitizing, or counting SERS events, can decrease the limit of detection in flowing solutions enabling quantification of single molecules. By using multivariate curve resolution and establishing a score threshold, each individual spectrum can be classified as containing an event or not. This binary "yes/no" can then be quantified, and a linear region can be established. This method was shown to lower the limit of detection to the lowest physical limit, and lowered the limit of detection by an order of magnitude from the traditional, intensity based LOD calculations.
表面增强拉曼散射(SERS)提供了一种无需标记的方法,可从多样且复杂的信号中分析分子,潜在地具有单分子灵敏度。SERS光谱固有的化学特异性能够识别分子;然而,由于等离子体环境的多样性而产生的信号变异性会限制定量分析,尤其是在低浓度情况下。在此我们表明,对SERS事件进行数字化或计数,可以降低流动溶液中的检测限,从而实现单分子的定量分析。通过使用多元曲线分辨并建立分数阈值,每个单独的光谱都可以被分类为是否包含一个事件。然后可以对这种二元的“是/否”进行量化,并建立一个线性区域。该方法被证明能将检测限降低到最低物理极限,并比基于传统强度的检测限计算方法将检测限降低了一个数量级。
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