Creating a regular array of metal-complexing molecules on an insulator surface at room temperature.
Creating a regular array of metal-complexing molecules on an insulator surface at room temperature.
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DOI：
10.1038/s41467-020-20189-x
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发表时间：
2020-12-21
影响因子：
16.6
通讯作者：
Kühnle A
中科院分区：
文献类型：
--
作者：
Aeschlimann S;Bauer SV;Vogtland M;Stadtmüller B;Aeschlimann M;Floris A;Bechstein R;Kühnle A
在室温下控制体绝缘体上的自组装纳米结构对于未来分子器件的制造至关重要，例如，在纳米电子学、催化和传感器应用领域。然而，在对于操作现实的温度下，将单个分子锚定在电绝缘支撑表面上仍然是一个很大的挑战。在这里，我们提出了一个有序阵列的形成单一的锚定分子，四乙酸二钼，在（10.4）平面的方解石（碳酸钙）。基于我们的原子力显微镜测量和密度泛函理论计算相结合的研究，我们表明，分子既不扩散，也不旋转，在室温下。强锚定是由一个理想的大小匹配的分子的静电相互作用解释。特别是在高覆盖率下，分子的硬球排斥和方解石表面的限制驱动分子形成局部有序阵列，这在概念上不同于金属有机框架中使用的有吸引力的连接体。我们的工作表明，定制的分子表面相互作用开辟了锚定单个金属络合分子有序阵列的可能性。在大块绝缘材料上有序排列的金属原子在光电子学和数据存储等领域有着广阔的应用前景。在这里，作者展示了一种基于金属络合分子的定制锚定和硬球排斥来创建有序金属阵列的策略。
Controlling self-assembled nanostructures on bulk insulators at room temperature is crucial towards the fabrication of future molecular devices, e.g., in the field of nanoelectronics, catalysis and sensor applications. However, at temperatures realistic for operation anchoring individual molecules on electrically insulating support surfaces remains a big challenge. Here, we present the formation of an ordered array of single anchored molecules, dimolybdenum tetraacetate, on the (10.4) plane of calcite (CaCO3). Based on our combined study of atomic force microscopy measurements and density functional theory calculations, we show that the molecules neither diffuse nor rotate at room temperature. The strong anchoring is explained by electrostatic interaction of an ideally size-matched molecule. Especially at high coverage, a hard-sphere repulsion of the molecules and the confinement at the calcite surface drives the molecules to form locally ordered arrays, which is conceptually different from attractive linkers as used in metal-organic frameworks. Our work demonstrates that tailoring the molecule-surface interaction opens up the possibility for anchoring individual metal-complexing molecules into ordered arrays. Arrays of ordered metal atoms on bulk insulating materials are promising for future applications, such as optoelectronics and data storage. Here, the authors demonstrate a strategy to create an ordered metal array based on tailored anchoring and hard-sphere repulsion of metal-complexing molecules.
影响因子：
3.1
作者：
Nony L;Bocquet F;Para F;Chérioux F;Duverger E;Palmino F;Luzet V;Loppacher C
通讯作者：
Loppacher C