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The development of organic artificial synapses that exhibit biomimicry features also may enable a more seamless integration of neuroelectronic devices in the nervous system, allowing artificial neuromodulation to be perceived as natural behavior by neuronal cells. Nevertheless, the capability to interact with both electroactive and non-electroactive neurotransmitters remains a challenge since state-of-the-art devices mainly rely on the oxidation of electroactive species. Here, the study proposes an organic artificial synapse engineered to enable interaction with non-electroactive species present in the central nervous system. By integrating a conductive polymeric film functionalized with platinum nanoparticles, the device can catalyze the oxidation of electroactive molecules (i.e., H 2 O 2 ) resulting from neurotransmitter-specific enzymatic reactions following an enzymatic functionalization, therefore exhibiting neuromorphic functions driven by non-electroactive neurotransmitters. The creation of devices that can interact with or monitor these neurotransmitters can be seen as a significant step toward innovative technologies to expand the understanding of the mechanisms underlying neurological disorders and the development of novel, more effective treatments for them., (© 2024 The Author(s). Advanced Materials published by Wiley‐VCH GmbH.)

Neurohybrid systems have gained large attention for their potential as in vitro and in vivo platform to interrogate and modulate the activity of cells and tissue within nervous system. In this scenario organic neuromorphic devices have been engineered as bioelectronic platforms to resemble characteristic neuronal functions. However, aiming to a functional communication with neuronal cells, material synthesis, and surface engineering can yet be exploited for optimizing bio-recognition processes at the neuromorphic-neuronal hybrid interface. In this work, artificial neuronal-inspired lipid bilayers have been assembled on an electrochemical neuromorphic organic device (ENODe) to resemble post-synaptic structural and functional features of living synapses. Here, synaptic conditioning has been achieved by introducing two neurotransmitter-mediated biochemical signals, to induce an irreversible change in the device conductance thus achieving Pavlovian associative learning. This new class of in vitro devices can be further exploited for assembling hybrid neuronal networks and potentially for in vivo integration within living neuronal tissues., (© 2024 The Authors. Advanced Science published by Wiley‐VCH GmbH.)

Synaptic plasticity is a fundamental process for neuronal communication and is involved in neurodegeneration. This process has been recently exploited to inspire the design of next-generation bioelectronic platforms. Neuromorphic devices have emerged as ideal candidates in mimicking brain functionalities, thanks to their ionic-to-electronic signal transduction, biocompatibility, and their ability to display short- and long-term memory as biological synapses. However, these devices still fail in bridging the gap between electronics and biological systems due to the lack of biomimetic features. Here, a biomembrane-based organic electrochemical transistor (OECT) is implemented and the supported-lipid-bilayer-mediated short-term depression of the device is investigated. After morphological and electrical characterization of the lipid bilayer, its ionic barrier behavior is exploited to enhance the neuromorphic operation of the OECT. Such biomimetic neuromorphic devices pave the way toward the implementation of synapses-resembling in vitro platforms to investigate and characterize neurodegenerative processes involving synaptic plasticity loss., (© 2022 The Authors. Advanced Materials published by Wiley-VCH GmbH.)