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Concentration Determination at a Countable Molecular Level in Nanofluidics by Solvent-Enhanced Photothermal Optical Diffraction
Analytical Chemistry ( IF 6.7 ) Pub Date : 2020-10-20 , DOI: 10.1021/acs.analchem.0c02024 Yoshiyuki Tsuyama 1 , Kazuma Mawatari 2
Analytical Chemistry ( IF 6.7 ) Pub Date : 2020-10-20 , DOI: 10.1021/acs.analchem.0c02024 Yoshiyuki Tsuyama 1 , Kazuma Mawatari 2
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Nanofluidic devices have become a powerful tool for extremely precise analyses at a single-molecule/nanoparticle level. However, a simple and sensitive molecular detection method is essential for nanofluidic devices because of ultrasmall volume (fL–aL). One such technology is photothermal spectroscopy (PTS), which utilizes light absorption and thermal relaxation by target molecules. Recently, we developed a photothermal optical diffraction (POD) detection method as PTS for nanofluidic devices. However, the detectable concentration range was in the order of μM (102 to 104 molecules), and further improvement in detection performance is strongly required. Here, we demonstrate solvent-enhanced POD with optimized experimental conditions and show its capability of concentration determination of nonfluorescent molecules in nanochannels at a countable molecular level. A relationship between the POD signal and thermal/optical properties of solvents is elucidated. We estimate the diffraction factor and photothermal factor of the solvent enhancement effect by thermal simulations and theoretical calculations. Experimental results show good agreement with the prediction, and the detection performance of the POD is successfully improved. At the optimized condition, we demonstrate the concentration determination with the limit of detection of 75 nM, which corresponds to an average of 10 molecules in a detection volume of 0.23 fL. Our sensitive nonfluorescent molecule detection method will be applied to a wide range of chemical/biological analyses utilizing nanofluidics.
中文翻译：
溶剂增强的光热光学衍射法测定纳米流体中可数分子水平的浓度
纳米流体设备已成为在单分子/纳米颗粒水平上进行极其精确的分析的强大工具。然而，由于超小体积（fL–aL），一种简单而灵敏的分子检测方法对于纳米流体设备至关重要。一种这样的技术是光热光谱法（PTS），其利用目标分子的光吸收和热弛豫。最近，我们开发了一种光热光学衍射（POD）检测方法作为纳米流体装置的PTS。但是，可检测的浓度范围约为μM（10 2到10 4分子），强烈要求进一步提高检测性能。在这里，我们展示了优化实验条件的溶剂增强型POD，并显示了其在可计数分子水平上确定纳米通道中非荧光分子浓度的能力。阐明了POD信号与溶剂的热/光学性质之间的关系。我们通过热模拟和理论计算来估计溶剂增强作用的衍射因子和光热因子。实验结果与预测结果吻合良好，成功地提高了POD的检测性能。在优化的条件下，我们证明了检测限为75 nM的浓度测定，这对应于检测体积为0的10个分子的平均值。23升 我们灵敏的非荧光分子检测方法将应用到利用纳米流体技术进行广泛的化学/生物学分析中。
更新日期：2020-11-03
中文翻译：
溶剂增强的光热光学衍射法测定纳米流体中可数分子水平的浓度
纳米流体设备已成为在单分子/纳米颗粒水平上进行极其精确的分析的强大工具。然而，由于超小体积（fL–aL），一种简单而灵敏的分子检测方法对于纳米流体设备至关重要。一种这样的技术是光热光谱法（PTS），其利用目标分子的光吸收和热弛豫。最近，我们开发了一种光热光学衍射（POD）检测方法作为纳米流体装置的PTS。但是，可检测的浓度范围约为μM（10 2到10 4分子），强烈要求进一步提高检测性能。在这里，我们展示了优化实验条件的溶剂增强型POD，并显示了其在可计数分子水平上确定纳米通道中非荧光分子浓度的能力。阐明了POD信号与溶剂的热/光学性质之间的关系。我们通过热模拟和理论计算来估计溶剂增强作用的衍射因子和光热因子。实验结果与预测结果吻合良好，成功地提高了POD的检测性能。在优化的条件下，我们证明了检测限为75 nM的浓度测定，这对应于检测体积为0的10个分子的平均值。23升 我们灵敏的非荧光分子检测方法将应用到利用纳米流体技术进行广泛的化学/生物学分析中。
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