“…Using organic molecules as the nanoscale building blocks, the concept of molecular selfassembly has become an integrated strategy for building molecular-based devices. [4][5][6] In general, the self-assembly process mainly relies on noncovalent interactions such as hydrogen bonding, [7][8][9] halogen bonding, [10][11][12][13] van der Waals interaction, [14][15][16] π-π interaction, [17][18][19] electrostatic interaction, [20][21][22] Exploring supramolecular architectures at surfaces plays an increasingly important role in contemporary science, especially for molecular electronics. A paradigm of research interest in this context is shifting from 2D to 3D that is expanding from monolayer, bilayers, to multilayers.…”