Nanoscience and Nanotechnology Research Center, Osaka Prefecture University, Sakai, Osaka 599-8570, Japan.
J Am Chem Soc. 2013 Mar 27;135(12):4592-5. doi: 10.1021/ja311463b. Epub 2013 Mar 18.
Understanding electron transfer (ET) from a single molecule to another single molecule holds essential importance to realize bottom-up molecular devices in which constituent molecules are self-assembled via noncovalent interactions between each other. However, rather little is currently known about the ET properties at the single-molecule interface. Here we employ molecular tips to quantify the ET through a H-bond between single molecules. We found that a H-bond conducts electrons better than a covalent σ bond at short-range. Its conductance, however, decays steeply as the chain length of the H-bonded molecules increases. First-principle calculations were performed to reveal the electronic origin of the facile ET through the H-bond. Our results demonstrate that H-bonding in a molecular junction significantly affects its transport property.
理解单个分子到另一个单个分子的电子转移(ET)对于实现自下而上的分子器件至关重要,其中组成分子通过彼此之间的非共价相互作用自组装。然而,目前对于单分子界面处的 ET 性质知之甚少。在这里,我们使用分子尖端通过单个分子之间的氢键来定量 ET。我们发现,在短程范围内,氢键比共价 σ 键更能传导电子。然而,随着氢键分子链长的增加,其电导急剧下降。我们进行了第一性原理计算,以揭示通过氢键进行的 ET 的容易发生的电子起源。我们的结果表明,分子结中的氢键会显著影响其传输性质。