Creating a regular array of metal-complexing molecules on an insulator surface at room temperature

Aeschlimann, Simon, Bauer, Sebastian V., Vogtland, Maximilian , Stadtmüller, Benjamin, Aeschlimann, Martin, Floris, Andrea, Bechstein, Ralf, Kühnle, Angelika, , and , (2020) Creating a regular array of metal-complexing molecules on an insulator surface at room temperature. Nature Communications, 11 (1). ISSN 2041-1723

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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.

Keywords:atomic force microscopy, bulk insulator, density functional calculations, entropy, metal array, nanostructures, self-assembly
Subjects:F Physical Sciences > F200 Materials Science
F Physical Sciences > F300 Physics
F Physical Sciences > F170 Physical Chemistry
F Physical Sciences > F343 Computational Physics
F Physical Sciences > F100 Chemistry
Divisions:College of Science > School of Chemistry
ID Code:43494
Deposited On:04 Jan 2021 12:00

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