Single Crystals of Perylene Diimide‐Based Two‐Dimensional Covalent Organic Frameworks

L Ling Zhang Z Zixuan Chen (State Key Laboratory of Analytical Chemistry for Life Science, School of Chemistry, School of Environment) L Lukas Mühlnickel (Institute of Applied Physics and Würzburg‐Dresden Cluster of Excellence ctd.qmat TUD Dresden University of Technology Dresden Germany) L Lukas Sporrer J Jakub D. Jasinski (Institute of Applied Physics and Würzburg‐Dresden Cluster of Excellence ctd.qmat TUD Dresden University of Technology Dresden Germany) M Megha Koottungal (Faculty of Chemistry and Food Chemistry TUD Dresden University of Technology Dresden Germany) K Kevin Synnatschke (Chair for Molecular Functional Materials, TU Dresden, Stadtgutstr. 59, 01217 Dresden, Germany) P Paul‐Felix Jordan (Faculty of Chemistry and Food Chemistry TUD Dresden University of Technology Dresden Germany) S Silvia Paasch (Faculty of Chemistry and Food Chemistry TUD Dresden University of Technology Dresden Germany) E Eike Brunner (Chair of Bioanalytical Chemistry) Z Zhehao Huang (Department of Chemistry) A Alexey Chernikov F Florian Auras (Cavendish Laboratory, Department of Physics)

Abstract

ABSTRACT Two‐dimensional covalent organic frameworks (2D COFs) are crystalline porous polymers with highly tunable structural and electronic properties. Although single crystals of these materials are highly desirable for fundamental research and potential applications, their synthesis has so far been limited to only a few examples. We have developed a high‐temperature double‐modulator synthetic strategy that enables the growth of single crystals from fully dissolved precursors. We applied this approach to generate a series of perylene diimide (PDI)‐based 2D COFs. These materials crystallize as platelets with lateral dimensions reaching up to 50 µm for the biphenyl‐linked PDI(Me) 8 ‐2P COF, providing a suitable platform for studying electronic processes via micro‐spectroscopy. Photoluminescence (PL) measurements revealed ultrafast monomer‐like emission together with a slower excimer‐related component. The availability of COF single crystals further enabled polarization‐dependent measurements, which revealed that the fast PL component is linearly polarized due to the parallel orientation of the PDI chromophores in the frameworks. These findings highlight the importance of COF single crystals for elucidating structure—photophysical property relationships of these intriguing materials.

Article Details

Volume / Issue Vol. 38, Issue 36
Published June 01, 2026
ISSN 0935-9648
Publisher Unknown Publisher

Journal Info

Advanced Materials

Unknown Publisher

ISSN: 0935-9648 Physical Sciences

Authors (13)

L

Ling Zhang

Z

Zixuan Chen

State Key Laboratory of Analytical Chemistry for Life Science, School of Chemistry, School of Environment

L

Lukas Mühlnickel

Institute of Applied Physics and Würzburg‐Dresden Cluster of Excellence ctd.qmat TUD Dresden University of Technology Dresden Germany

L

Lukas Sporrer

J

Jakub D. Jasinski

Institute of Applied Physics and Würzburg‐Dresden Cluster of Excellence ctd.qmat TUD Dresden University of Technology Dresden Germany

M

Megha Koottungal

Faculty of Chemistry and Food Chemistry TUD Dresden University of Technology Dresden Germany

K

Kevin Synnatschke

Chair for Molecular Functional Materials, TU Dresden, Stadtgutstr. 59, 01217 Dresden, Germany

P

Paul‐Felix Jordan

Faculty of Chemistry and Food Chemistry TUD Dresden University of Technology Dresden Germany

S

Silvia Paasch

Faculty of Chemistry and Food Chemistry TUD Dresden University of Technology Dresden Germany

E

Eike Brunner

Chair of Bioanalytical Chemistry

Z

Zhehao Huang

Department of Chemistry

A

Alexey Chernikov

F

Florian Auras

Cavendish Laboratory, Department of Physics