Exploiting the light–matter interplay to realize advanced light responsive multimodal platforms is an emerging strategy to engineer bioinspired systems such as optoelectronic synaptic devices. However, existing neuroinspired optoelectronic devices rely on complex processing of hybrid materials which often do not exhibit the required features for biological interfacing such as biocompatibility and low Young’s modulus. Recently, organic photoelectrochemical transistors (OPECTs) have paved the way towards multimodal devices that can better couple to biological systems benefiting from the characteristics of conjugated polymers. Neurohybrid OPECTs can be designed to optimally interface neuronal systems while resembling typical plasticity-driven processes to create more sophisticated integrated architectures between neuron and neuromorphic ends. Here, an innovative photo-switchable PEDOT:PSS was synthesized and successfully integrated into an OPECT. The OPECT device uses an azobenzene-based organic neuro-hybrid building block to mimic the retina’s structure exhibiting the capability to emulate visual pathways. Moreover, dually operating the device with opto- and electrical functions, a light-dependent conditioning and extinction processes were achieved faithful mimicking synaptic neural functions such as short- and long-term plasticity.

Over the last few years, organic bioelectronics has experienced an exponential growth with applications encompassing platforms for tissue engineering, drug delivery systems, implantable, and wearable sensors. Although reducing the physical and mechanical mismatch with the human tissues allows to increase the coupling efficiency, several challenges are still open in terms of matching biological curvature, size, and interface stiffness. In this context, the replacement of bulky with more flexible and conformable devices is required, implying the transition from inorganic conventional electronics to organic electronics. Indeed, the advent of organic materials in bioelectronics, due to the indisputable benefits related to biocompatibility, flexibility, and electrical properties, has granted superior coupling properties with human tissues increasing the performances of both sensing and stimulation platforms. In this review the ease of functionalization and patterning of conductive polymers (CPs) will be analyzed as a strategy that enables the fabrication of platforms with high structural flexibility ranging from the macro to the micro/nano‐scales, leading to the increase of devices sensitivity. Drawing from the concept of biomimicry, the human body tissues interfaces will be explored through an ideal journey starting from organic platforms for epidermal sensing and stimulation. Then, devices capable of establishing a dynamic coupling with the heart will be reviewed and finally, following the circulatory system and crossing the blood‐brain barrier, the brain will be reached and novel sensing and computing implants advances that pave the way to the possibility to emulate as well as to interact with the neural functions will be analyzed.

Organic neuromorphic platforms have recently received growing interest for the implementation and integration of artificial and hybrid neuronal networks. Here, achieving closed-loop and learning/training processes as in the human brain is still a major challenge especially exploiting time-dependent biosignalling such as neurotransmitter release. Here, we present an integrated organic platform capable of cooperating with standard silicon technologies, to achieve brain-inspired computing via adaptive synaptic potentiation and depression, in a closed-loop fashion. The microfabricated platform could be interfaced and control a robotic hand which ultimately was able to learn the grasping of differently sized objects, autonomously.

The electrolyte used in dye-sensitized solar cells (DSSCs) plays a key role in the process of current generation, and hence the analysis of charge-transfer mechanisms both in its bulk and at its interfaces with other materials is of fundamental importance. Because of solvent confinement, gel polymer electrolytes are more practical and convenient to use with respect to liquid electrolytes, but in-depth studies are still necessary to optimize their performances. In this work, gel polymer electrolytes of general formulation polyacrylonitrile (PAN)/ethylene carbonate (EC)/propylene carbonate (PC)/MI, where M⁺ is a cation in the alkaline series Li–Cs, were prepared and used in DSSCs. Their ionic conductivities were determined by impedance analysis, and their temperature dependence showed Arrhenius behavior within the experimental window. FT-IR studies of the electrolytes confirmed the prevalence of EC coordination around the cations. Photo-anodes were prepared by adsorbing organic sensitizer D35 on nanocrystalline TiO₂ thin films, and employed to build DSSCs with the gel electrolytes. Nanosecond transient spectroscopy results indicated a slightly faster dye regeneration process in the presence of large cations (Cs⁺, Rb⁺). Moreover, a negative shift of TiO₂ flat-band potential with the decreasing charge density of the cations (increasing size) was observed through Mott–Schottky analysis. In general, results indicate that cell efficiencies are mostly governed by photocurrent values, in turn depending on the conductivity increase with cation size. Accordingly, the best result was obtained with the Cs⁺-containing cell, although in this case a slight reduction of photovoltage compared to Rb⁺ was observed.