Robust Organic Radical Molecular Junctions Using Acetylene Terminated Groups for C-Au Bond Formation
Robust Organic Radical Molecular Junctions Using Acetylene Terminated Groups for C-Au Bond Formation
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DOI：
10.1021/jacs.7b10019
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发表时间：
2018-02-07
影响因子：
15
通讯作者：
Crivillers, Nuria
中科院分区：
文献类型：
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作者：
Bejarano, Francesc;Olavarria-Contreras, Ignacio Jose;Crivillers, Nuria
有机顺磁分子和电活性分子作为分子电子和自旋电子器件的核心元件引起了人们的兴趣。目前，进一步的进展受到分子/电极接触的适度稳定性和再现性的阻碍。我们报告的持久性有机自由基轴承一个和两个末端炔基形成Au-C σ键的合成。研究了室温下自组装单分子膜的形成、稳定性和单分子结的电子输运。对两个系统的综合分析表明，与传统的硫基连接体相比，这种连接体与金形成了牢固的共价键，并且形成了更好的接触。密度泛函理论和量子输运计算支持的实验观察，突出了减少的可变性的电导值的C-Au基结。我们的发现推进了对基于电活性分子的设备的鲁棒性和再现性的追求。
Organic paramagnetic and electroactive molecules are attracting interest as core components of molecular electronic and spintronic devices. Currently, further progress is hindered by the modest stability and reproducibility of the molecule/electrode contact. We report the synthesis of a persistent organic radical bearing one and two terminal alkyne groups to form Au-C sigma bonds. The formation and stability of self-assembled monolayers and the electron transport through single-molecule junctions at room temperature have been studied. The combined analysis of both systems demonstrates that this linker forms a robust covalent bond with gold and a better-defined contact when compared to traditional sulfur-based linkers. Density functional theory and quantum transport calculations support the experimental observation highlighting a reduced variability of conductance values for the C-Au based junction. Our findings advance the quest for robustness and reproducibility of devices based on electroactive molecules.