Single-Molecule Tunneling Sensors for Nitrobenzene Explosives,Analytical Chemistry

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Single-Molecule Tunneling Sensors for Nitrobenzene Explosives
Analytical Chemistry ( IF 6.7 ) Pub Date : 2022-08-15 , DOI: 10.1021/acs.analchem.2c01592
Peikai Yu ₁ , Lichuan Chen ₁ , Yanxi Zhang ₁ , Shiqiang Zhao ₁ , Zhixin Chen ₁ , Yong Hu ₁ , Junyang Liu ₁ , Yang Yang ₁ , Jia Shi ₁ , Zhiyi Yao ₂ , Wenjing Hong ₁

Affiliation

The tunneling current through the single-molecule junctions principally offers the ultimate solution for chemical and biochemical sensing via the interactions between probes and target analytes at the single-molecule level. However, it remains unexplored to achieve the sensitive and selective detection of targeted analytes using single-molecule junction techniques due to the challenge in quantitative evaluation of sensing sensitivity and selectivity. Herein, we demonstrate a single-molecule tunneling sensor for the highly sensitive and selective detection of nitrobenzene explosives using scanning tunneling microscope break junction (STM-BJ). Taking advantage of π–π stacking interactions between the molecular probes and nitrobenzene explosives, we use a spectral clustering algorithm to assign the signal of probes and π-stacked probes for sensitively detecting the targeted analytes and the distinguishable conductance change of probes when interacting with different nitroaromatic explosive compounds for selective detection. We find that pronounced conductance changes up to 0.8 orders of magnitude when the probes interact with TNT. Also, we obtain a sensitivity of up to ∼10 pM for TNT and high sensitivity for eight TNT analogues. Combined with theoretical calculations, we discover that the harness of the destructive quantum interference of the probe M1OH after interacting with TNT leads to high selectivity in sensing with TNT. Our work demonstrates the great potential of the single-molecule tunneling current for environmental sensing molecules with high selectivity and sensitivity.

中文翻译：

用于硝基苯炸药的单分子隧道传感器

通过单分子结的隧穿电流主要通过探针和目标分析物在单分子水平上的相互作用为化学和生化传感提供最终解决方案。然而，由于在传感灵敏度和选择性的定量评估方面存在挑战，使用单分子结技术实现对目标分析物的灵敏和选择性检测仍未得到探索。在此，我们展示了一种单分子隧道传感器，用于使用扫描隧道显微镜断裂结 (STM-BJ) 对硝基苯炸药进行高灵敏度和选择性检测。利用分子探针和硝基苯炸药之间的 π-π 堆积相互作用，我们使用光谱聚类算法分配探针和 π-stacked 探针的信号，用于灵敏检测目标分析物，以及探针与不同硝基芳烃化合物相互作用时可区分的电导变化进行选择性检测。我们发现当探针与 TNT 相互作用时，显着的电导变化高达 0.8 个数量级。此外，我们对 TNT 获得了高达 ~10 pM 的灵敏度，对八种 TNT 类似物获得了高灵敏度。结合理论计算，我们发现探针M1OH与TNT相互作用后的破坏性量子干涉的利用导致TNT传感的高选择性。我们的工作证明了单分子隧穿电流对于具有高选择性和灵敏度的环境传感分子的巨大潜力。

更新日期：2022-08-15

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