Controlled Migration of Lithium Cations by Diamine Bridges in Water‐Processable Polymer‐Based Solid‐State Electrolyte Memory Layers for Organic Synaptic Transistors

Synaptic transistors require sufficient retention (memory) performances of current signals to exactly mimic biological synapses. Ion migration has been proposed to achieve high retention characteristics but less attention has been paid to polymer-based solid-state electrolytes (SSEs) for organic synaptic transistors (OSTRs). Here, OSTRs with water-processable polymer-based SSEs, featuring ion migration-controllable molecular bridges, which are prepared by reactions of poly(4-styrenesulfonic acid) (PSSA), diethylenetriamine (DETA), and lithium hydroxide (LiOH) are demonstrated. The ion conductivity of PSSA:LiOH:DETA (1:0.4:X, PLiD) films is remarkably changed by the molar ratio (X) of DETA, which is attributed to the extended distances between the PSSA chains by the DETA bridges. The devices with the PLiD layers deliver noticeably changed hysteresis reaching an optimum at X = 0.2, leading to the longest retention of current signals upon single/double pulses. The long-term potentiation test confirms that the present OSTRs can gradually build up the postsynaptic current by gate pulses of -2 V, while the long-term depression can be adjusted by varying the depression gate pulses (≈0.2-1.2 V). The artificial neural network simulations disclose that the present OSTRs with the ion migration-controlled PLiD layers can perform synaptic processes with an accuracy of ≈96%.