Mechanistic Insights into Layered Growth of Imine-Linked Bilayer 2D Covalent Organic Frameworks

The purpose of this dataset is to provide readers with access to the experimental data used in the publication “Mechanistic Insights into Layered Growth of Imine-Linked Bilayer 2D Covalent Organic Frameworks” (DOI: 10.1021/jacs.5c19958). This folder contains a dataset of scanning tunneling microscopy (STM) and atomic force microscopy (AFM) images, as well as a U-Net script for STM image analysis. In this work, an imine-linked bilayer two-dimensional covalent organic framework (2D COF) was synthesized using 1,3,5-tris(4-aminophenyl)benzene (TAPB) and 1,3,5-tris(p-formylphenyl)benzene (TFPB) with a fixed TAPB:TFPB molar ratio of 1:1 at the liquid/solid interface (octanoic acid/HOPG interface). STM imaging reveals a layered growth mechanism involving defect-mediated nucleation, lattice-guided directional propagation, cross-defect growth, and oriented domain coalescence. This growth pathway gives rise to locally ordered-on-disordered stacking embedded within predominantly AA-stacking domains.