Michelle Ernst^1*, Jürg Hutter^2*, Stefano Battaglia^2*

1 Institute of Geological Sciences, University of Bern, Baltzerstrasse 1+3, 3012 Bern, Switzerland

2 Department of Chemistry, University of Zurich, 8057 Zürich, Switzerland

* Corresponding authors emails: michelle.ernst@unibe.ch, hutter@chem.uzh.ch, stefano.battaglia@chem.uzh.ch

DOI10.24435/materialscloud:yw-3f [version v1]

Publication date: Apr 22, 2025

How to cite this record

Michelle Ernst, Jürg Hutter, Stefano Battaglia, Extensive band gap tunability in covalent organic frameworks via metal intercalation and high pressure, Materials Cloud Archive 2025.63 (2025), https://doi.org/10.24435/materialscloud:yw-3f

Description

Covalent organic frameworks (COFs) are materials of growing interest for electronic applications due to their tunable structures, chemical stability, and layered architectures that support extended π-systems and directional charge transport. While their electronic properties are strongly influenced by the choice of molecular building blocks and the stacking arrangement, experimental control over these features remains limited, and the number of well-characterized COFs is still relatively small. Here, we explore two alternative strategies, hydrostatic pressure and metal intercalation, to tune the electronic structure of COFs. Using periodic density functional theory (DFT) calculations, we show that the band gap of pristine COF-1 decreases by ∼1 eV under compression up to 10 GPa. Metal intercalation induces an even greater reduction, in some cases leading to metallic behavior. We demonstrate that pressure and intercalation offer effective, continuous control over COF electronic properties, providing powerful means to complement and extend conventional design approaches.

Materials Cloud sections using this data

Files

File name	Size	Description
MaterialsCloudArchive.tar.gz MD5md5:4e4683ca2ffe48736b8ab1f58c4552b4	53.4 MiB	Inputs and output of CP2K calculations sorted by COF and pressure.

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External references

Keywords

MARVEL Swiss National Supercomputing Center (CSCS) covalent-organic frameworks DFT electronic bands band gap high pressure intercalation