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DOE OSTI · 3010086

Supramolecular Control of Ionic Retention in Electrolyte-Gated Synaptic Transistors

Zhou, Haolei [Cornell Univ., Ithaca, NY (United States)]·Chivukula, Kaushik [Cornell Univ., Ithaca, NY (United States)]·Fang, Qiyi [Cornell Univ., Ithaca, NY (United States)]·Wang, Kaiyang [Cornell Univ., Ithaca, NY (United States)] (ORCID:0000000215290958)·Ren, Xinyi [Cornell Univ., Ithaca, NY (United States)]·Garudapalli, Ashutosh [Cornell Univ., Ithaca, NY (United States)] (ORCID:0000000223402083)·Liang, Ce [Univ. of Chicago, IL (United States)] (ORCID:0000000180851558)·Tian, Jinpeng [Princeton Univ., NJ (United States)]·Butler, Satya [Princeton Univ., NJ (United States)] (ORCID:0009000577825443)·Liang, Anke [Cornell Univ., Ithaca, NY (United States)]·Xu, Jason [Cornell Univ., Ithaca, NY (United States)]·Zhang, Honghu [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000317847825)·Xie, Saien [Princeton Univ., NJ (United States)]·Yeo, Jingjie [Cornell Univ., Ithaca, NY (United States)] (ORCID:0000000264627422)·Zhong, Yu [Cornell Univ., Ithaca, NY (United States)] (ORCID:0000000186312213)
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Abstract

Electrolyte-gated transistors with ion-trapping layers offer a promising platform for artificial synapses in neuromorphic computing, yet molecular mechanisms governing ionic retention remain poorly understood. Here, in this study, we present a supramolecular approach to modulate ion retention by incorporating a crown ether derivative-based polymer network as an ion-trapping layer on top of a semiconducting monolayer. We show that the balance between ion–host binding and ion–solvent interactions dictates the kinetics of ion capture and release, which in turn controls the memory characteristics of the device. By varying the solvent dielectric constant, we tune the ionic retention time from nearly permanent trapping to rapid relaxation. Intermediate solvent polarity enables programmable short- and long-term synaptic behaviors, including excitatory postsynaptic current, paired-pulse facilitation, and long-term potentiation and depression. These findings establish a direct link between supramolecular ion recognition and synaptic plasticity and provide a generalizable design strategy for ionic–electronic neuromorphic devices.

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36 MATERIALS SCIENCE

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Zhou, Haolei [Cornell Univ., Ithaca, NY (United States)], Chivukula, Kaushik [Cornell Univ., Ithaca, NY (United States)], Fang, Qiyi [Cornell Univ., Ithaca, NY (United States)], Wang, Kaiyang [Cornell Univ., Ithaca, NY (United States)] (ORCID:0000000215290958), Ren, Xinyi [Cornell Univ., Ithaca, NY (United States)], Garudapalli, Ashutosh [Cornell Univ., Ithaca, NY (United States)] (ORCID:0000000223402083), Liang, Ce [Univ. of Chicago, IL (United States)] (ORCID:0000000180851558), Tian, Jinpeng [Princeton Univ., NJ (United States)], Butler, Satya [Princeton Univ., NJ (United States)] (ORCID:0009000577825443), Liang, Anke [Cornell Univ., Ithaca, NY (United States)], Xu, Jason [Cornell Univ., Ithaca, NY (United States)], Zhang, Honghu [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000317847825), Xie, Saien [Princeton Univ., NJ (United States)], Yeo, Jingjie [Cornell Univ., Ithaca, NY (United States)] (ORCID:0000000264627422), Zhong, Yu [Cornell Univ., Ithaca, NY (United States)] (ORCID:0000000186312213). 2025-12-03. Supramolecular Control of Ionic Retention in Electrolyte-Gated Synaptic Transistors. https://doi.org/10.1021/acsmaterialslett.5c01336

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36 MATERIALS SCIENCE↗