Small‐Molecule Mixed Ionic‐Electronic Conductors for Efficient N‐Type Electrochemical Transistors: Structure‐Function Correlations

Cho, Yongjoon; Gao, Lin; Yao, Yao; Kim, Jaehyun; Zhang, Dayong; Forti, Giacomo; Duplessis, Isaiah; Wang, Yuyang; Pankow, Robert M.; Ji, Xudong; Rivnay, Jonathan; Marks, Tobin J.; Facchetti, Antonio

doi:10.1002/ange.202414180

Small‐Molecule Mixed Ionic‐Electronic Conductors for Efficient N‐Type Electrochemical Transistors: Structure‐Function Correlations

Journal Article · Sat Nov 02 00:00:00 EDT 2024 · Angewandte Chemie

DOI:https://doi.org/10.1002/ange.202414180· OSTI ID:2475899

Cho, Yongjoon ^[1]; Gao, Lin ^[1]; Yao, Yao ^[1]; Kim, Jaehyun ^[1]; Zhang, Dayong ^[1]; Forti, Giacomo ^[1]; Duplessis, Isaiah ^[2]; Wang, Yuyang ^[1]; Pankow, Robert M. ^[1]; Ji, Xudong ^[3]; Rivnay, Jonathan ^[3]; Marks, Tobin J. ^[1]; ^[4]

Department of Chemistry Northwestern University 2145 Sheridan Road Evanston IL 60208–3113 USA
Department of Materials Science and Engineering Northwestern University 2145 Sheridan Road Evanston IL 60208–3113 USA
Department of Biomedical Engineering Northwestern University 2145 Sheridan Road Evanston IL 60208–3113 USA
Department of Chemistry Northwestern University 2145 Sheridan Road Evanston IL 60208–3113 USA, School of Materials Science and Engineering Georgia Institute of Technology Atlanta GA 30332 USA

Abstract

The fundamental challenge in electron‐transporting organic mixed ionic‐electronic conductors (OMIECs) is simultaneous optimization of electron and ion transport. Beginning from Y6‐type/U‐shaped non‐fullerene solar cell acceptors, we systematically synthesize and characterize molecular structures that address the aforementioned challenge, progressively introducing increasing numbers of oligoethyleneglycol (OEG; g) sidechains from 1 g to 3 g, affording OMIECs 1gY, 2gY, and 3gY, respectively. The crystal structure of 1gY preserves key structural features of the Y n series: a U‐shaped/planar core, close π–π molecular stacking, and interlocked acceptor groups. Versus inactive Y6 and Y11, all of the new glycolated compounds exhibit mixed ion‐electron transport in both conventional organic electrochemical transistor (cOECT) and vertical OECT (vOECT) architectures. Notably, 3gY with the highest OEG density achieves a high transconductance of 16.5 mS, an on/off current ratio of ~10 ⁶ , and a turn‐on/off response time of 94.7/5.7 ms in vOECTs. Systematic optoelectronic, electrochemical, architectural, and crystallographic analysis explains the superior 3gY‐based OECT performance in terms of denser n gY OEG content, increased crystallite dimensions with decreased long‐range crystalline order, and enhanced film hydrophilicity which facilitates ion transport and efficient redox processes. Finally, we demonstrate an efficient small‐molecule‐based complementary inverter using 3gY vOECTs, showcasing the bioelectronic applicability of these new small‐molecule OMIECs.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-05CH11231; AC02-06CH11357

OSTI ID:: 2475899

Journal Information:: Angewandte Chemie, Journal Name: Angewandte Chemie; ISSN 0044-8249

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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Small‐Molecule Mixed Ionic‐Electronic Conductors for Efficient N‐Type Electrochemical Transistors: Structure‐Function Correlations

Journal Article · Sat Nov 02 00:00:00 EDT 2024 · Angewandte Chemie (International Edition) · OSTI ID:2475900

Small‐Molecule Mixed Ionic‐Electronic Conductors for Efficient N‐Type Electrochemical Transistors: Structure‐Function Correlations

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