Simulation of interlayer coupling for electroactive covalent organic framework design

Porous, stacked two-dimensional covalent organic frameworks (2D COFs) bearing semiconducting linkers can support directional charge transfer across adjacent layers of the COF. To better inform the current and possible future design rules for enhancing electron and hole transport in such materials, a...

Full description

Saved in:
Bibliographic Details
Published in:The Journal of chemical physics 2024-05, Vol.160 (18)
Main Authors: Leo, Tanner M., Robbins, Megan, Sullivan, Alana, Thornes, Henry, Fitzsimmons, Garrett, Goodey, Alyssa, Kowalczyk, Tim
Format: Article
Language:English
Subjects:
Carrier transport
Charge transfer
Couplings
Current carriers
Electronic structure
Interlayers
Molecular dynamics
Potential energy
Citations: Items that this one cites
Online Access:Get full text
Tags: Add Tag
No Tags, Be the first to tag this record!
Description
Summary:Porous, stacked two-dimensional covalent organic frameworks (2D COFs) bearing semiconducting linkers can support directional charge transfer across adjacent layers of the COF. To better inform the current and possible future design rules for enhancing electron and hole transport in such materials, an understanding of how linker selection and functionalization affects interlayer electronic couplings is essential. We report electronic structure simulation and analysis of electronic couplings across adjacent linker units and to encapsulated species in functionalized electroactive 2D COFs. The detailed dependence of these electronic couplings on interlayer interactions is examined through scans along key interlayer degrees of freedom and through configurational sampling from equilibrium molecular dynamics on semiempirical potential energy surfaces. Beyond affirming the sensitivity of the electronic coupling to interlayer distance and orientation, these studies offer guidance toward linker functionalization strategies for enhancing charge carrier transport in electroactive 2D COFs.
ISSN:0021-9606
1089-7690
DOI:10.1063/5.0206246