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PreprintCC BYChemRxiv

Cation Coordination as a Molecular Handle to Program Synaptic behavior in OrganicMemristors

  1. 1University of Valencia
  2. 2Trinity College Dublin

Abstract

Organic mixed ionic-electronic conductors offer a route to soft, low-voltage neuromorphic electronics because ionic motion can directly modulate electronic conductance, providing a materials-level analogue of synaptic plasticity.However, the molecular origin of this ion-electron coupling remains poorly understood, limiting the rational design of artificial synapses for time-dependent tasks such as visual recognition.Here, we show that synaptic dynamics in Organic mixed ionic-electronic memristors can be programmed by chemically controlling salt dissociation within the active matrix.The devices combine Super Yellow, alkali-metal triflate salts (XOTf; X = Li, Na or K), and trimethylolpropane ethoxylate, an oligoether that coordinates the cations with different strengths.This coordination regulates the voltage-dependent population of mobile triflate anions available to compensate holes injected into Sy, thereby controlling electrochemical p-doping and the memristive response.As a result, cation identity systematically tunes the activation threshold, ON/OFF ratio, switching kinetics, relaxation dynamics and volatility.Under pulsed stimulation, these programmed ion dynamics enable short-term and long-term plasticity, as well as spike-timing-dependent plasticity, with conductanceupdate amplitudes following the trend SyLi > SyNa > SyK.Learning rules extracted from the devices were implemented in spiking neural-network simulations for digit recognition, yielding accuracies of 87%, 86% and 76% for SyLi, SyNa and SyK, respectively, after one training epoch using 1000 MNIST images.This corresponds to a 60-fold reduction in training data relative to the full MNIST benchmark commonly used in neuromorphic simulations.These results link molecular control of salt dissociation to programmable ion-electron coupling, enabling efficient organic synapses for time-resolved neuromorphic vision.

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BibTeX
@misc{gonzalezcervera2026cation,
  title = {{Cation Coordination as a Molecular Handle to Program Synaptic behavior in OrganicMemristors}},
  author = {Laura González-Cervera and Javier Alda and Silvia Gimenez-Santamaria and Joaquin Soriano-Lopez and Roger Sanchis-Gual and Ramón Torres-Cavanillas and Eugenio Coronado},
  howpublished = {ChemRxiv},
  year = {2026},
  month = sep,
  doi = {10.26434/chemrxiv.15008624/v1},
  url = {https://chemrxiv.org/doi/full/10.26434/chemrxiv.15008624/v1},
  note = {CC BY},
}
RIS
TY  - UNPB
TI  - Cation Coordination as a Molecular Handle to Program Synaptic behavior in OrganicMemristors
AU  - Laura González-Cervera
AU  - Javier Alda
AU  - Silvia Gimenez-Santamaria
AU  - Joaquin Soriano-Lopez
AU  - Roger Sanchis-Gual
AU  - Ramón Torres-Cavanillas
AU  - Eugenio Coronado
PY  - 2026
DA  - 2026/09/10
PB  - ChemRxiv
DO  - 10.26434/chemrxiv.15008624/v1
UR  - https://chemrxiv.org/doi/full/10.26434/chemrxiv.15008624/v1
AB  - Organic mixed ionic-electronic conductors offer a route to soft, low-voltage neuromorphic electronics because ionic motion can directly modulate electronic conductance, providing a materials-level analogue of synaptic plasticity.However, the molecular origin of this ion-electron coupling remains poorly understood, limiting the rational design of artificial synapses for time-dependent tasks such as visual recognition.Here, we show that synaptic dynamics in Organic mixed ionic-electronic memristors can be programmed by chemically controlling salt dissociation within the active matrix.The devices combine Super Yellow, alkali-metal triflate salts (XOTf; X = Li, Na or K), and trimethylolpropane ethoxylate, an oligoether that coordinates the cations with different strengths.This coordination regulates the voltage-dependent population of mobile triflate anions available to compensate holes injected into Sy, thereby controlling electrochemical p-doping and the memristive response.As a result, cation identity systematically tunes the activation threshold, ON/OFF ratio, switching kinetics, relaxation dynamics and volatility.Under pulsed stimulation, these programmed ion dynamics enable short-term and long-term plasticity, as well as spike-timing-dependent plasticity, with conductanceupdate amplitudes following the trend SyLi > SyNa > SyK.Learning rules extracted from the devices were implemented in spiking neural-network simulations for digit recognition, yielding accuracies of 87%, 86% and 76% for SyLi, SyNa and SyK, respectively, after one training epoch using 1000 MNIST images.This corresponds to a 60-fold reduction in training data relative to the full MNIST benchmark commonly used in neuromorphic simulations.These results link molecular control of salt dissociation to programmable ion-electron coupling, enabling efficient organic synapses for time-resolved neuromorphic vision.
ER  -