TY - JOUR
T1 - High-Performance Organic Electrochemical Transistors and Neuromorphic Devices Comprising Naphthalenediimide-Dialkoxybithiazole Copolymers Bearing Glycol Ether Pendant Groups
AU - Zhang, Yanxi
AU - Ye, Gang
AU - van der Pol, Tom P.A.
AU - Dong, Jingjing
AU - van Doremaele, Eveline R.W.
AU - Krauhausen, Imke
AU - Liu, Yuru
AU - Gkoupidenis, Paschalis
AU - Portale, Giuseppe
AU - Song, Jun
AU - Chiechi, Ryan C.
AU - van de Burgt, Yoeri
N1 - Funding Information:
Y.Z., E.R.W.v.D., and Y.v.d.B. gratefully acknowledge funding from the European Union's Horizon 2020 Research and Innovation Programme, grant agreement no. 802615. G.Y. and J.S. acknowledge the National Natural Science Foundation of China (61620106016/61835009/61775145). G.Y. also acknowledges the China Postdoctoral Science Foundation Funded Project (grant 2020M672771) and Guangdong Basic and Applied Basic Research Foundation (2020A1515110636). T.P.A.v.d.P. acknowledges funding from the Netherlands Ministry of Education, Culture and Science (Gravity program 024.001.035). G.P. acknowledges the Zernike Institute for Advanced Materials for the startup funds. J.D. and G.P. are grateful to the China Scholarship Council (CSC No. 201606340158). Y.v.d.B., I.K., and P.G. acknowledge funding for a joint project between the Max Planck Institute of Polymer Research and the Institute for Complex Molecular Systems (ICMS), Eindhoven University of Technology, grant no. MPIPICMS2019001.
Publisher Copyright:
© 2022 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH.
PY - 2022/7/4
Y1 - 2022/7/4
N2 - Organic electrochemical transistors (OECTs) have emerged as building blocks for low power circuits, biosensors, and neuromorphic computing. While p-type polymer materials for OECTs are well developed, the choice of high-performance n-type polymers is limited, despite being essential for cation and metabolite biosensors, and crucial for constructing complementary circuits. N-type conjugated polymers that have efficient ion-to-electron transduction are highly desired for electrochemical applications. In this contribution, three non-fused, planar naphthalenediimide (NDI)-dialkoxybithiazole (2Tz) copolymers, which systematically increase the amount of polar tri(ethylene glycol) (TEG) side chains: PNDI2OD-2Tz (0 TEG), PNDIODTEG-2Tz (1 TEG), PNDI2TEG-2Tz (2 TEG), are reported. It is demonstrated that the OECT performance increases with the number of TEG side chains resulting from the progressively higher hydrophilicity and larger electron affinities. Benefiting from the high electron mobility, excellent ion conduction capability, efficient ion-to-electron transduction, and low-lying lowest unoccupied molecular orbital energy level, the 2 TEG polymer achieves close to 105 on-off ratio, fast switching, 1000 stable operation cycles in aqueous electrolyte, and has a long shelf life. Moreover, the higher number TEG chain substituted polymer exhibits good conductance state retention over two orders of magnitudes in electrochemical resistive random-access memory devices, highlighting its potential for neuromorphic computing.
AB - Organic electrochemical transistors (OECTs) have emerged as building blocks for low power circuits, biosensors, and neuromorphic computing. While p-type polymer materials for OECTs are well developed, the choice of high-performance n-type polymers is limited, despite being essential for cation and metabolite biosensors, and crucial for constructing complementary circuits. N-type conjugated polymers that have efficient ion-to-electron transduction are highly desired for electrochemical applications. In this contribution, three non-fused, planar naphthalenediimide (NDI)-dialkoxybithiazole (2Tz) copolymers, which systematically increase the amount of polar tri(ethylene glycol) (TEG) side chains: PNDI2OD-2Tz (0 TEG), PNDIODTEG-2Tz (1 TEG), PNDI2TEG-2Tz (2 TEG), are reported. It is demonstrated that the OECT performance increases with the number of TEG side chains resulting from the progressively higher hydrophilicity and larger electron affinities. Benefiting from the high electron mobility, excellent ion conduction capability, efficient ion-to-electron transduction, and low-lying lowest unoccupied molecular orbital energy level, the 2 TEG polymer achieves close to 105 on-off ratio, fast switching, 1000 stable operation cycles in aqueous electrolyte, and has a long shelf life. Moreover, the higher number TEG chain substituted polymer exhibits good conductance state retention over two orders of magnitudes in electrochemical resistive random-access memory devices, highlighting its potential for neuromorphic computing.
KW - ethylene glycol side chains
KW - neuromorphic devices
KW - non-fused donor-acceptor conjugated polymers
KW - organic electrochemical transistors
UR - http://www.scopus.com/inward/record.url?scp=85127603020&partnerID=8YFLogxK
U2 - 10.1002/adfm.202201593
DO - 10.1002/adfm.202201593
M3 - Article
AN - SCOPUS:85127603020
SN - 1616-301X
VL - 32
JO - Advanced Functional Materials
JF - Advanced Functional Materials
IS - 27
M1 - 2201593
ER -