Single-Molecule Junction Formation in Deep Eutectic Solvents with Highly Effective Gate Coupling.
Single-Molecule Junction Formation in Deep Eutectic Solvents with Highly Effective Gate Coupling.
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DOI：
10.1021/acs.jpcc.3c03129
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发表时间：
2023-07-06
影响因子：
3.7
通讯作者：
Nichols, Richard J.
中科院分区：
文献类型：
--
作者：
Qiao, Xiaohang;Vezzoli, Andrea;Smith, Shaun;Higgins, Simon J.;Davidson, Ross J.;Beeby, Andrew;Nichols, Richard J.
分子连接周围的环境会影响其电荷传输特性，因此必须谨慎选择。在液体介质中进行测量的情况下，溶剂必须提供良好的溶剂化作用，赋予结稳定性，并且在电解质浇注实验的情况下，通过控制双电层允许与栅电极的有效电耦合。我们在这项研究中评估了低共熔溶剂混合物 (DES) 乙醇，它是氯化胆碱和乙二醇 (1:2) 的混合物，用于通过断裂连接技术制造单分子连接。在乙醇中，我们能够（i）利用 DES 提供的改进的溶剂化能力来测量具有挑战性和难溶性的分子线，以及（ii）有效地应用能够在 ~1 V 电位窗口内将结的电导调节大约一个数量级的静电门。 Au-VDP-Au 结上的电化学选通结果非常好地遵循具有强栅极耦合的单级建模（其中 VDP 是 1,2-二（吡啶-4-基）乙烯）。乙醇也是测量非常短的分子连接的理想溶剂，因为它可以在点接触破裂时大大缩短金属电极的回弹距离。我们的工作表明，DES 是通常相对昂贵的离子液体的可行替代品，为单分子电学测量提供了良好的多功能性。
The environment surrounding a molecular junction affects its charge-transport properties and, therefore, must be chosen with care. In the case of measurements in liquid media, the solvent must provide good solvation, grant junction stability, and, in the case of electrolyte gating experiments, allow efficient electrical coupling to the gate electrodes through control of the electrical double layer. We evaluated in this study the deep eutectic solvent mixture (DES) ethaline, which is a mixture of choline chloride and ethylene glycol (1:2), for single-molecule junction fabrication with break-junction techniques. In ethaline, we were able to (i) measure challenging and poorly soluble molecular wires, exploiting the improved solvation capabilities offered by DESs, and (ii) efficiently apply an electrostatic gate able to modulate the conductance of the junction by approximately an order of magnitude within a ∼1 V potential window. The electrochemical gating results on a Au–VDP–Au junction follow exceptionally well the single-level modeling with strong gate coupling (where VDP is 1,2-di(pyridine-4-yl)ethene). Ethaline is also an ideal solvent for the measurement of very short molecular junctions, as it grants a greatly reduced snapback distance of the metallic electrodes upon point-contact rupture. Our work demonstrates that DESs are viable alternatives to often relatively expensive ionic liquids, offering good versatility for single-molecule electrical measurements.
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