Notice
This is not the latest version of this item. The latest version can be found at: https://repository.kaust.edu.sa/handle/10754/663432
Ion Coordination and Chelation in a Glycolated Polymer Semiconductor: Molecular Dynamics and X-Ray Fluorescence Study
Name:
Ion_Coordination_and_Chelation_in_a_Glycolated_Polymer_Semiconductor__Molecular_Dynamics_and_X-Ray_Fluorescence_Study_v2.pdf
Size:
8.964Mb
Format:
PDF
Type
PreprintAuthors
Matta, Micaela
Wu, Ruiheng
Paulsen, Bryan D.
Petty, Anthony
Sheelamanthula, Rajendar
McCulloch, Iain

Schatz, George C

Rivnay, Jonathan
KAUST Department
KAUST Solar Center (KSC)Chemical Science Program
Physical Science and Engineering (PSE) Division
Date
2020-05-08Permanent link to this record
http://hdl.handle.net/10754/663432.1
Metadata
Show full item recordAbstract
Organic electrochemical transistors (OECTs) are based on the doping of a semiconducting polymer by an electrolyte. Due to their ability to conjugate volumetric ion penetration with high hole mobility and charge density, polythiophenes bearing glycolated side chains have rapidly surged as the highest performing materials for OECTs; amongst them, p(g2T-TT) is amongst those with the highest figure of merit. While recent studies have shown how different doping anions tend to affect the polymer microstructure, only a handful of electrolytes have been tested in mixed conduction devices. Our work provides an atomistic picture of the p(g2T-TT) -electrolyte interface in the ‘off’ state of an OECT, expected to be dominated by cation-polymer interactions. Using a combination of molecular dynamics simulations and X-ray fluorescence, we show how different anions effectively tune the coordination and chelation of cations by glycolated polymers. At the same time, softer and hydrophobic anions such as TFSI and ClO$_{4}$ are found to preferentially interact with the p(g2T-TT) phase, further enhancing polymer-cation coordination. Besides opening the way for a full study of electrolyte doping mechanisms in operating devices, our results suggest that tailoring the electrolyte for different applications and materials might be a viable strategy to tune the performance of mixed conducting devices.Citation
Matta, M., Wu, R., Paulsen, B. D., Petty, A., Sheelamanthula, R., McCulloch, I., … Rivnay, J. (2020). Ion Coordination and Chelation in a Glycolated Polymer Semiconductor: Molecular Dynamics and X-Ray Fluorescence Study. doi:10.26434/chemrxiv.12264308.v1Sponsors
M.M. is grateful to Prof. Alessandro Troisi for useful comments during the preparation of this manuscript. R.W. and B.D.P. are grateful to Dr. Christos D. Malliakas for helpful discussion.Publisher
American Chemical Society (ACS)ae974a485f413a2113503eed53cd6c53
10.26434/chemrxiv.12264308.v1
Scopus Count
Except where otherwise noted, this item's license is described as Archived with thanks to American Chemical Society (ACS)