One of the major limitations of standard top‐down technologies used in today's neuromorphic engineering is their inability to map the 3D nature of biological brains. Here, it is shown how bipolar electropolymerization can be used to engineer 3D networks of PEDOT:PSS dendritic fibers. By controlling the growth conditions of the electropolymerized material, it is investigated how dendritic fibers can reproduce structural plasticity by creating structures of controllable shape. Gradual topologies evolution is demonstrated in a multielectrode configuration. A detailed electrical characterization of the PEDOT:PSS dendrites is conducted through DC and impedance spectroscopy measurements and it is shown how organic electrochemical transistors (OECT) can be realized with these structures. These measurements reveal that quasi‐static and transient response of OECTs can be adjusted by controlling dendrites’ morphologies. The unique properties of organic dendrites are used to demonstrate short‐term, long‐term, and structural plasticity, which are essential features required for future neuromorphic hardware development.

Although materials and processes are different from biological cells’, brain mimicries led to tremendous achievements in parallel information processing via neuromorphic engineering. Inexistent in electronics, we emulate dendritic morphogenesis by electropolymerization in water, aiming in operando material modification for hardware learning. Systematic study of applied voltage-pulse parameters details on tuning independently morphological aspects of micrometric dendrites’: fractal number, branching degree, asymmetry, density or length. Growths time-lapse image processing shows spatial features to be dynamically dependent, and expand distinctively before and after conductive bridging with two electro-generated dendrites. Circuit-element analysis and impedance spectroscopy confirms their morphological control in temporal windows where growth kinetics is finely perturbed by the input frequency and duty cycle. By the emulation of one’s most preponderant mechanisms for brain’s long-term memory, its implementation in vicinity of sensing arrays, neural probes or biochips shall greatly optimize computational costs and recognition required to classify high-dimensional patterns from complex environments.

Electropolymerization is a bottom-up materials engineering process of micro/nano-scale that utilizes electrical signals to deposit conducting dendrites morphologies by a redox reaction in the liquid phase. It resembles synaptogenesis in the brain, in which the electrical stimulation in the brain causes the formation of synapses from the cellular neural composites. The strategy has been recently explored for neuromorphic engineering by establishing link between the electrical signals and the dendrites’ shapes. Since the geometry of these structures determines their electrochemical properties, understanding the mechanisms that regulate polymer assembly under electrically programmed conditions is an important aspect. In this manuscript, we simulate this phenomenon using mesoscale simulations, taking into account the important features of spatial–temporal potential mapping based on the time-varying signal, the motion of charged particles in the liquid due to the electric field, and the attachment of particles on the electrode. The study helps in visualizing the motion of the charged particles in different electrical conditions, which is not possible to probe experimentally. Consistent with the experiments, the higher AC frequency of electrical activities favors linear wire-like growth, while lower frequency leads to more dense and fractal dendrites’ growth, and voltage offset leads to asymmetrical growth. We find that dendrites' shape and growth process systematically depend on particle concentration and random scattering. We discover that the different dendrites’ architectures are associated with different Laplace and diffusion fields, which govern the monomers’ trajectory and subsequent dendrites’ growth. Such unconventional engineering routes could have a variety of applications from neuromorphic engineering to bottom-up computing strategies.

The brain capitalizes on the complexity of both its biochemistry for neurons to encode diverse pieces of information with various neurotransmitters and its morphology at multiple scales to route different pathways for neural interconnectivity. Conducting polymer dendrites can show similar features by differentiating between cations and anions thanks to their charge accumulation profile and the asymmetry in their dendriticity that allows projecting spike signals differently. Here, we exploit such mimicry for in materio classification of bursting activity and investigate, in phosphate buffered saline, the capability of such object to sense bursts of voltage pulses of 100 mV amplitude, emitted by a local gate in the vicinity of the dendrite. The dendrite integrates the different activities with a fading memory time window that is characteristic of both the polarity of the spikes and the temporality of the burst. By this first demonstration, the "material-object" definitely shows great potential to be a node halfway between the two realms of brain and electronic communication.