High Iontronic Performance in Organic Electrochemical Transistors Enabled by Intramolecular Noncovalent Interactions.

Liu, Guocai; Zhang, Meng; Lv, Jikai; Wang, Hao; Ma, Bowei; Gu, Xiaobin; Guo, Yunlong; Liu, Yunqi et al. · Adv Mater · 2026

basic_science · Level V

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Abstract

Organic electrochemical transistors (OECTs) show great potential in bioelectronics due to their iontronic coupling, low driving voltages (<1 V), and biocompatibility. Nevertheless, their low iontronic performance, particularly in terms of transconductance (g<sub>m</sub>), limits their ability to acquire high-precision biosignals. To address this issue, a series of poly(bithiophene)s (opg2T-O, opg2T-S, and opg2T-Se) bearing 4,4'-position glycol side chains are synthesized. Upon varying furan, thiophene, and selenophene comonomers, the intramolecular noncovalent interactions are systematically tuned. Comprehensive theoretical analyses reveal that opg2T-Se demonstrates stronger intramolecular Se···O noncovalent interactions than the S···O interactions in opg2T-S and opg2T-O, affording a more planar and rigid molecular configuration in opg2T-Se. Meanwhile, opg2T-Se exhibits closer π-π stacking and lamellar-packing and prefers an edge-on orientation. Consequently, a record-high geometry-normalized transconductance (g<sub>m,n</sub>) of 415 S cm<sup>-1</sup>, along with remarkable hole mobility (µ = 2.99 cm<sup>2</sup> V<sup>-1</sup> s<sup>-1</sup>) and volumetric capacitance (C* = 423.3 F cm<sup>-3</sup>) are achieved in opg2T-Se based OECTs. Importantly, the opg2T-Se-based devices exhibits much higher signal fidelity in in-vitro human electrocardiogram (ECG) than the other two devices. This study highlights the importance of intramolecular noncovalent interaction in the channel layer materials for achieving high-performance OECTs.