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Area of Science:

  • Surface Chemistry
  • Supramolecular Chemistry
  • Materials Science

Background:

  • Chemical synthesis typically favors ordered structures.
  • On-surface synthesis usually produces linear, ordered 2D networks.
  • Generating 2D random networks via on-surface synthesis has been a challenge.

Purpose of the Study:

  • To demonstrate the fabrication of a 2D random network using on-surface synthesis.
  • To explore the controlled formation of convoluted 1D stripes into a 2D network.
  • To investigate the potential of this method for creating advanced supramolecular hosts.

Main Methods:

  • On-surface synthesis on a Cu(111) surface.
  • Utilizing 4,4',5,5'-tetrabromodibenzo[18]crown-6 ether (BrCR) precursors.
  • Employing Ullmann reaction conditions with controlled intermediate states.
  • Characterization via ultrahigh vacuum low-temperature scanning tunneling microscopy and spectroscopy (UHV-LT-STM/STS).
  • Theoretical analysis using density functional theory (DFT) calculations.

Main Results:

  • Successful synthesis of a 2D random network of convoluted stripes from BrCR precursors.
  • Demonstration that adjusting intermediate state quantities controls network topology.
  • Observation of stripe formation facilitated by the crown ether precursor's structure and Ullmann coupling.
  • Detailed understanding of growth mechanisms and electronic properties through STM/STS and DFT.

Conclusions:

  • On-surface synthesis can be leveraged to create 2D random networks, not just ordered structures.
  • The method allows for the construction of complex, winding 2D networks by controlling precursor bonding.
  • This provides a new pathway for designing advanced ring host supramolecules with enhanced guest capture capabilities.