发表机构
University of Cambridge; University of Oxford; Princeton University（剑桥大学; 牛津大学; 普林斯顿大学）
机构由 AI 辅助整理，请以论文原文为准。AI 中文总结
本研究针对有机混合离子-电子导体（OMIECs）偏置移除后电荷弛豫规律不明的问题，采用原位电荷光度法结合建模与冷冻电镜分析，揭示其电荷弛豫机制，通过调控聚噻吩侧链实现稳定存储或快速传感的不同应用。
AI 中文摘要
有机混合离子-电子导体（OMIECs）可耦合离子与电子信号，适用于能量存储、神经形态计算及生物电子学领域。然而，偏置移除后电荷在水中的弛豫规律（该规律决定存储状态的持续时长）仍不明确。本研究采用原位电荷光度法，追踪OMIEC薄膜在偏置及开路弛豫过程中的电荷变化：偏置状态下，电荷以氧化还原前沿形式移动；偏置移除后，电荷转而在沟道内均匀弛豫。建模与冷冻电镜分析表明，溶胀作用会在材料本体中形成连通的富水通道，这类通道可加快离子运动，但也会导致存储电荷泄漏。通过调控聚噻吩的末端侧链可控制水的吸收量与离子捕获能力： bulky疏水侧链可实现稳定的可编程状态，而亲水侧链则支持快速电生理传感。
英文摘要
Organic mixed ionic-electronic conductors (OMIECs) couple ionic and electronic signals, enabling energy storage, neuromorphic computing, and bioelectronics. However, how charge relaxes in water once the bias is removed, which determines how long stored states persist, remains unclear. Using operando charge photometry, we tracked charge in OMIEC films during biasing and open-circuit relaxation. Under bias, charges moved as redox fronts. After bias removal, charge instead relaxed uniformly across the channel. Modeling and cryo-electron microscopy indicate that swelling creates connected water-rich pathways through the bulk. These pathways speed ion motion but also let stored charge leak away. Tuning the terminal side chain of a polythiophene controls water uptake and ion trapping. Bulky hydrophobic side chains enable stable programmable states, whereas hydrophilic side chains support fast electrophysiology sensing.
Comments17 pages, 5 figures
