Quantitative Microscopic Observation of Base?Ligand Interactions via Hydrogen Bonds by Single-Molecule Counting
Quantitative Microscopic Observation of Base?Ligand Interactions via Hydrogen Bonds by Single-Molecule Counting
复制标题
通过单分子计数定量显微观察氢键碱基配体相互作用
DOI：
10.1021/jacs.2c11260
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发表时间：
2023
影响因子：
15
通讯作者：
Taniguchi Masateru
中科院分区：
文献类型：
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作者：
Takashima Yusuke;Komoto Yuki;Ohshiro Takahito;Nakatani Kazuhiko;Taniguchi Masateru
自引入阿伏加德罗数以来，化学性质一直以统计平均值为基础。缺乏合适的方法来计数已识别的单分子，这给计数统计学带来了挑战。组成DNA的碱基和小分子之间的选择性、亲和力和氢键方式对生物体至关重要，目前还没有在单分子水平上揭示出来。在这里，我们展示了基于单分子电学测量和人工智能相结合的单分子计数对上述参数的量化。通过测定碱基分子与配体混合溶液中聚集体数目的比值，定量地评价了五种配体与四种不同碱基分子的结合选择性。此外，我们还通过单分子计数和量子化学计算，揭示了微观氢键的模式和数目与配体的关系。
Chemical properties have been based on statistical averages since the introduction of Avogadro’s number. The lack of suitable methods for counting identified single molecules has posed challenges to counting statistics. The selectivity, affinity, and mode of hydrogen bonding between base and small molecules that make up DNA, which is vital for living organisms, have not yet been revealed at the single molecule level. Here, we show the quantitation of the above-mentioned parameters via single-molecule counting based on the combination of single-molecule electrical measurements and AI. The binding selectivity values of five ligands to four different base molecules were evaluated quantitatively by determining the ratio of the number of aggregates in a solution mixture of base molecules and a ligand. In addition, we show the ligand dependence of the mode and number of microscopic hydrogen bonds via single-molecule counting and quantum chemical calculations.