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. 2025 Jul 7;37(14):5226-5233.
doi: 10.1021/acs.chemmater.5c00949. eCollection 2025 Jul 22.

Molar Mass Improves the Performance of n‑Type Organic Electrochemical Transistors

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Molar Mass Improves the Performance of n‑Type Organic Electrochemical Transistors

Dominik Stegerer et al. Chem Mater. .

Abstract

We report on the synthesis and use of two side-chain-free ionenes with varying heteroatoms, PFu and PTh, for n-type accumulation-mode OECTs. Compared to PTh, PFu is more challenging to make, less stable, and shows increased water solubility. The optical properties and surface morphologies of the two derivatives are comparable, but their microstructures vary distinctly in terms of ordering and backbone orientation. While the backbones of PTh show a preferential face-on orientation, PFu is significantly less ordered. The OECT performance of PTh is improved by 1 order of magnitude compared to PFu, as indicated by μC* values of 116.16 and 10.66 F cm-1 V-1 s-1, respectively. Further increasing the molar mass of PTh doubles the performance, resulting in a record-high μC* value of 225.71 F cm-1 V-1 s-1 and a high μ value of 0.58 cm2 V-1 s-1, highlighting the crucial role of molecular weight control for enhancing device performance.

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Figures

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1. Chemical Structures of PTh and PFu
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1H NMR spectra (selected regions) of the (a) monomer, (b,c) nonquaternized polymers, (d) quaternized monomer, and (e,f) quaternized polymers. (g,h) Enlarged regions with details of end-group analysis. SEH: silyl ether hydrolysis.
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UV–vis spectra of the polymers in (a) D2O and (b) thin films. (c) Cyclic voltammograms of the reduction process of the polymers in thin films on ITO-coated substrates. The dashed lines indicate reduction potentials used to calculate the LUMO energy levels.
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1D and 2D GIWAXS patterns of thin films of (a) PFu, (b) PTh, and (c) PTh-HMW. (d) In-plane and (e) out-of-plane 1D GIWAXS line cuts of the three samples.
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(a) Transfer characteristics and (b) geometry-normalized transconductance of the OECTs. (c–e) Output characteristics of PFu-, PTh-, and PTh-HMW-based OECTs, respectively. All OECTs had the same channel geometry (W = 10 μm, L = 10 μm, and d = 30 nm). (f) Graphical comparison of material performance parameters (μC* vs. μ) with literature data.

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