Chemical Research in Chinese Universities ›› 2025, Vol. 41 ›› Issue (5): 1037-1047.doi: 10.1007/s40242-025-5076-y

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Thermal Annealing-modulated Ion Doping and Synaptic Behavior of Organic Electrochemical Transistors Based on Block Copolymers

XIANG Chuan1, JIANG Xingyu1, Li Bin1, JIANG Jichao2, WANG Qi1, SHI Cheng1, DONG Xinyu1, LIU Dianjue1, XUE Di1, ZHANG Jidong2, HUANG Lizhen1, CHI Lifeng1   

  1. 1. Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-based Functional Materials & Devices, Soochow University, Suzhou 215123, P. R. China;
    2. Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, P. R. China
  • Received:2025-04-22 Accepted:2025-07-06 Online:2025-10-01 Published:2025-09-26
  • Contact: CHI Lifeng, E-mail: chilf@suda.edu.cn;HUANG Lizhen, E-mail: lzhuang@suda.edu.cn E-mail:chilf@suda.edu.cn;lzhuang@suda.edu.cn
  • Supported by:
    This work was supported by the National Natural Science Foundation of China (Nos. 22222205, 52173176), the Fund of the Suzhou Key Laboratory of Surface and Interface Intelligent Matter, China (No. SZS2022011), the Fund of the Collaborative Innovation Center of Suzhou Nano Science & Technology, the Priority Academic Program Development (PAPD) of Jiangsu Higher Education Institutions, China, and the ‘111’ Project.

Abstract: Organic electrochemical transistors (OECTs) garner significant attention in biosensing and neuromorphic computing applications owing to their high transconductance, low operating voltage, and biocompatibility. Among the various factors influencing OECTs performance and functionality, particularly synaptic behavior emulation, ion doping/dedoping kinetics play a pivotal role. However, precise control of ion dynamics remains challenging because of the complex interplay between material properties and microstructural characteristics. In this study, we demonstrate the modulation of the ion doping dynamics and synaptic behavior of OECTs based on hydrophilic-hydrophobic block copolymers (DPP-b-g2T-T) through thermal annealing. We investigate the correlations among segmental hydrophilicity/hydrophobicity, crystallinity, and ion transport kinetics. Our findings reveal that hydrophilic g2T-T segments enhance the ion doping efficiency, whereas hydrophobic DPP segments restrict ion transport. Thermal annealing reduces the ion doping/dedoping rates for both segments, particularly Au-gated OECTs. This phenomenon is attributed to the enhanced film crystallinity, which impedes ion transport, especially under the relatively weak gate control effect characteristic of Au. Leveraging the annealing-modulated ion doping/dedoping dynamics and prolonged retention time, we emulate short-term plasticity (STP) and long-term plasticity (LTP). This work establishes a strategy for optimizing OECTs synaptic performance through synergistic molecular design and thermal annealing, contributing to the advancement of neuromorphic technology.

Key words: Organic electrochemical transistor, Hydrophilic-hydrophobic block copolymer, Thermal annealing, Ion transport dynamics, Synaptic plasticity