Simulation of interlayer coupling for electroactive covalent organic framework design

Area of Science:

• Materials Science
• Computational Chemistry
• Organic Electronics

Background:

• Two-dimensional covalent organic frameworks (2D COFs) with semiconducting linkers enable directional charge transfer between layers.
• Optimizing charge transport in these materials necessitates understanding the influence of linker selection and functionalization on electronic couplings.

Purpose of the Study:

• To investigate how linker functionalization affects interlayer electronic couplings in electroactive 2D COFs.
• To provide design rules for enhancing electron and hole transport in 2D COFs.

Main Methods:

• Electronic structure simulations were performed to analyze electronic couplings.
• Interlayer interactions were examined through systematic scans of degrees of freedom and molecular dynamics simulations on semiempirical potential energy surfaces.

Main Results:

• Electronic couplings are highly sensitive to interlayer distance and orientation.
• Specific linker functionalization strategies can significantly enhance charge carrier transport.

Conclusions:

• The study provides critical insights into the relationship between molecular design and charge transport properties in 2D COFs.
• Findings offer practical guidance for developing advanced 2D COFs for efficient electronic applications.