Single-Molecule Topochemical Analyses for Large-Scale Multiplexing Tasks
Single-Molecule Topochemical Analyses for Large-Scale Multiplexing Tasks
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DOI：
10.1021/acs.analchem.9b02483
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发表时间：
2019-11-05
影响因子：
7.4
通讯作者：
Mao, Hanbin
中科院分区：
文献类型：
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作者：
Mandal, Shankar;Zhang, Xiaoqing;Mao, Hanbin
多任务处理是下一代化学或生物分析的关键特征。然而，同时分析很少超过三个不同的任务，这归因于容纳分析单元的空间有限，以及随着任务数量的增加而降低的信噪比(S/N)水平。在这里，利用单分子技术的优势S/N，我们通过在DNA模板中对纳米分辨率的miRNA识别单元进行空间编码，同时在几秒钟内解码分析物结合，分析了五个microRNA生物标志物。发夹茎被内部环点缀，以编码miRNA的识别单元。通过发夹的机械展开，顺序地询问各个内部环是否与每个miRNA结合。利用这种所谓的拓扑化学时空分析，我们能够实现miRNAs的亚皮下摩尔检测下限。我们预计，这种新的单分子拓扑化学分析可以大规模分析单分子靶标。
Multitasking is the pivotal feature in next-generation chemo- or bioanalyses. However, simultaneous analyses rarely exceed over three different tasks, which is ascribed to the limited space to accommodate analyzing units and the compromised signal-to-noise (S/N) level as the number of tasks increases. Here, by leveraging superior S/N of single-molecule techniques, we analyzed five microRNA biomarkers by spatially encoding miRNA recognition units with nanometers resolution in a DNA template, while decoding the analyte binding temporally in seconds. The hairpin stem is interspersed by internal loops to encode recognition units for miRNA. By mechanical unfolding of the hairpin, individual internal loops are sequentially interrogated for the binding of each miRNA. Using this so-called topochemical spatiotemporal analysis, we were able to achieve subpicomolar detection limits of miRNAs. We anticipate that this new single-molecule topochemical analysis can massively analyze single-molecule targets.