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Covalently Doped and Highly Oriented Covalent Organic Framework Thin Films.

Dayanni D Bhagwandin^1,2, Brian M Everhart^1,3, Kirt A Page^1,2,4

¹Materials and Manufacturing Directorate, Air Force Research Laboratory, WPAFB, Ohio 45433, United States.

|July 10, 2025

Summary

Researchers developed a method to control the properties of 2D covalent organic frameworks (COFs) for microelectronics. Covalently doping COF thin films with thiophene linkers improved their electronic properties, acting as a p-type dopant.

Keywords:

band structure engineering covalent organic framework nanostructures semiconductors sulfur heterocycles thin films

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Microfluidic-based Synthesis of Covalent Organic Frameworks COFs: A Tool for Continuous Production of COF Fibers and Direct Printing on a Surface

Microfluidic-based Synthesis of Covalent Organic Frameworks COFs: A Tool for Continuous Production of COF Fibers and Direct Printing on a Surface

Published on: July 10, 2017

Area of Science:

Materials Science
Organic Chemistry
Solid-State Physics

Background:

2D covalent organic frameworks (COFs) are promising for microelectronics but challenging to process into thin films due to insolubility.
Controlling crystallographic orientation and band structure is key for high-performance COF-based devices.

Purpose of the Study:

To develop a strategy for controlled covalent doping of imine COF thin films.
To investigate the effect of thiophene linker incorporation on COF crystallinity and electronic properties.

Main Methods:

Liquid-solid synthesis of COF thin films using varying ratios of terephthalaldehyde (PDA) and 2,5-thiophenedicarboxaldehyde (TDA) with 1,3,5-tris(4-aminophenyl)benzene (TAPB).
Characterization of crystallographic ordering, band gap, work function, and valence band maximum.

Main Results:

Highly crystalline and uniformly oriented TAPB-PDA-TDA COF thin films were successfully synthesized with up to 20% TDA incorporation.
Thiophene doping minimally disrupted crystallographic ordering while reducing the band gap and increasing the work function.
Covalent doping enhanced π-conjugation and electron delocalization, demonstrating p-type semiconductor behavior.

Conclusions:

Controlled covalent doping of 2D COF thin films with thiophene linkers is achievable.
This doping strategy offers a pathway to tune the electronic properties of COFs for advanced microelectronic applications.
Enhanced crystallinity and π-conjugation in doped COFs improve charge transport properties.