Shape control in 2D molecular nanosheets by tuning anisotropic intermolecular interactions and assembly kinetics

Maximilian Dreher, Pierre Martin Dombrowski, Matthias Wolfgang Tripp, Niels Münster, Ulrich Koert and Gregor Witte ()
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Maximilian Dreher: Philipps-Universität Marburg
Pierre Martin Dombrowski: Philipps-Universität Marburg
Matthias Wolfgang Tripp: Philipps-Universität Marburg
Niels Münster: Philipps-Universität Marburg
Ulrich Koert: Philipps-Universität Marburg
Gregor Witte: Philipps-Universität Marburg

Nature Communications, 2023, vol. 14, issue 1, 1-9

Abstract: Abstract Since molecular materials often decompose upon exposure to radiation, lithographic patterning techniques established for inorganic materials are usually not applicable for the fabrication of organic nanostructures. Instead, molecular self-organisation must be utilised to achieve bottom-up growth of desired structures. Here, we demonstrate control over the mesoscopic shape of 2D molecular nanosheets without affecting their nanoscopic molecular packing motif, using molecules that do not form lateral covalent bonds. We show that anisotropic attractive Coulomb forces between partially fluorinated pentacenes lead to the growth of distinctly elongated nanosheets and that the direction of elongation differs between nanosheets that were grown and ones that were fabricated by partial desorption of a complete molecular monolayer. Using kinetic Monte Carlo simulations, we show that lateral intermolecular interactions alone are sufficient to rationalise the different kinetics of structure formation during nanosheet growth and desorption, without inclusion of interactions between the molecules and the supporting MoS2 substrate. By comparison of the behaviour of differently fluorinated molecules, experimentally and computationally, we can identify properties of molecules with regard to interactions and molecular packing motifs that are required for an effective utilisation of the observed effect.

Date: 2023
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DOI: 10.1038/s41467-023-37203-7

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