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Construction and Systematical Symmetric Studies of a Series of Supramolecular Clusters with Binary or Ternary Ammonium Triphenylacetates
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A 2D Substitutional Solid Solution through Hydrogen Bonding of Molecular Building Blocks.

Jennifer M MacLeod1, Josh Lipton-Duffin1, Chaoying Fu2

  • 1Institut National de la Recherche Scientifique, Centre Énergie, Matériaux, Télécommunications , 1650 Lionel Boulet Boulevard, Varennes, QC, Canada J3X 1S2.

ACS Nano
|August 15, 2017
PubMed
Summary

Researchers created a new 2D crystalline self-assembled molecular system using large, C3-symmetric molecules. This system shows substitutional disorder, forming a stable crystal lattice with randomly incorporated molecules, offering insights into entropy in molecular crystals.

Keywords:
entropyhydrogen bondingscanning tunneling microscopyself-assemblysolid solution

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Area of Science:

  • Supramolecular Chemistry
  • Materials Science
  • Surface Science

Background:

  • Two-dimensional (2D) molecular self-assembly yields ordered supramolecular layers.
  • Random intermixing and entropy typically lead to crystalline disorder or glassy phases in such systems.

Purpose of the Study:

  • To investigate the formation of a crystalline 2D self-assembled molecular system with substitutional disorder.
  • To understand the role of entropy and intermolecular interactions in creating such a structure.

Main Methods:

  • Utilized a mixture of trimesic acid (TMA) and terthienobenzenetricarboxylic acid (TTBTA) for self-assembly on highly oriented pyrolitic graphite (HOPG).
  • Employed Monte Carlo simulations to analyze the entropy of intermixing.
  • Applied density functional theory (DFT) calculations to determine the enthalpy of intermixing.

Main Results:

  • A 2D crystalline lattice was formed from TMA and TTBTA molecules of significantly different sizes.
  • TTBTA molecules substituted into the TMA lattice at a fixed stoichiometry of approximately 12%.
  • The lattice constant followed Vegard's law, and the lattice exhibited epitaxial alignment with the HOPG substrate.

Conclusions:

  • Demonstrated the formation of a randomly intermixed yet crystalline 2D solid through hydrogen bonding.
  • Highlighted the interplay of epitaxy, intermolecular forces, and entropy in molecular crystal formation.
  • Provided insights into the manifestation of entropy in confined molecular systems.