Abstract: In the quest to change the way we envision computing, the ability to create connections in between computing nodes on demand offers the very exciting possibility to explore bottom-up strategies when it comes to thinking the design of electronic devices a nd circuits. Recently, the growth of conductive polymer fibers via electropolymerization (most notably poly(3,4-ethylenedioxythiophene) doped with poly(styrenesulfonate), abbreviated as PEDOT:PSS) was employed in the realm of neuromorphic hardware, first as a way to tune the resistance of a connection, and then to perform computing tasks, such as biosignal classification trough reservoir computing, thus establishing the advantages of the method.In this work, we propose to demonstrate that electropolymer ization is a useful tool for the creation of sensors that are able to realize computing tasks in an aqueous environment. By taking advantage of the morphology of the fibers, we show that PEDOT:PSS dendrites can discriminate between different types of vol tage pulses emitted in their vicinity by a local gate electrode, thus performing in materio classification.In addition, we discuss the growth of networks of polymer fibers on 2D substrates. The ability to create structures that cover several microelectro des allows us to study the behavior of the whole system instead of a single dendrite, and it highlights the relationship that relates the morphology of the object and its electrical properties. In particular, we show that dendrites present an asymmetric non-linear behavior due to the volume of polymer that increases the capacitance of the device albeit not participating in conduction. Moreover, because of the ionoelectronic coupling that exists within an electrolyte, two active devices working concomita ntly will influence one another. We demonstrate that it is a blessing for the realization of computing tasks, such as logic, and that it can also be used to program the dendrites into non-volatile conductance states. Therefore, dendritic networks could c onstitute a new building block for non-conventional information processing that fits into the larger framework of brain-inspired computing.
Scholaert C., Janzakova K., Coffinier Y., Pecqueur S., Alibart F.
Abstract: Neuromorphic computing and engineering is capitalizing heavily on the new physical properties offered by nantechnologies to engineer biological processes. At the frontiers in between bio-mimetism and bio-inspiration, various solutions have been proposed for synaptic plasticity or neuronal features based on discrete memory elements, bistable switches or transistors circuits. One missing element that has been missing in the neuromorphic toolbox is the ability to reproduce the complex 3D interconnections o bserved in biological neural networks. Here, we propose to take advantage of bipolar electropolymerization of PEDOT dendritic fibers to reproduce the ability of neural networks to generate complex topologies. The electropolymerization mechanism is used t o realize structural plasticity based on Hebbian-like plasticity rules. We explore how such bottom-up process can find optimal topologies for specific computing tasks. We demonstrate that such optimal topologies results in a drastic reduction of intercon nects for classification and reconstruction tasks, thus offering an interesting option for neural network design.
Alibart F., Janzakova K., Scholaert C., Balafrej I., Kumar A., Drouin D., Rouat J., Pecqueur S., Coffinier Y.
Abstract: Neural networks are powerful tools for solving complex problems, but finding the right network topology for a given task remains an open question. Biology uses neurogenesis and structural plasticity to solve this problem. Advanced neural network algorith ms are mostly relying on synaptic plasticity and learning. The main limitation in reconciling these two approaches is the lack of a viable hardware solution that could reproduce the bottom-up development of biological neural networks. Here, we show how t he dendritic growth of PEDOT:PSS-based fibers through AC electropolymerization can implement structural plasticity during network development. We find that this strategy follows Hebbian principles and is able to define topologies that leverage better com puting performances with sparse synaptic connectivity for solving non-trivial tasks. This approach is validated in software simulation, and offers up to 61% better network sparsity on classification and 50% in signal reconstruction tasks.
Janzakova K., Balafrej I., Kumar A., Garg N., Scholaert C., Rouat J., Drouin D., Coffinier Y., Pecqueur S., Alibart F.*
Abstract: In the quest to change the way we envision computing, the ability to create connections in between computing nodes on demand offers the very exciting possibility to explore bottom-up strategies when it comes to thinking the design of electronic devices a nd circuits. Recently, the growth of conductive polymer fibers via electropolymerization (most notably poly(3,4-ethylenedioxythiophene) doped with poly(styrenesulfonate), abbreviated as PEDOT:PSS) was employed in the realm of neuromorphic hardware, first as a way to tune the resistance of a connection, and then to perform computing tasks, such as biosignal classification trough reservoir computing, thus establishing the advantages of the method. In this work, we propose to demonstrate that electropolyme rization is a useful tool for the creation of sensors that are able to realize computing tasks in an aqueous environment. By taking advantage of the morphology of the fibers, we show that PEDOT:PSS dendrites can discriminate between different types of vo ltage pulses emitted in their vicinity by a local gate electrode, thus performing in materio classification. In addition, we discuss the growth of networks of polymer fibers on 2D substrates. The ability to create structures that cover several microelect rodes allows us to study the behavior of the whole system instead of a single dendrite. Complex interactions through iono-electronic coupling arise when several fibers are interconnected. These mechanisms (e.g. self- / inter-gating, ionic relaxation,...) offer new possibilities for computing signals and could potentially open the way for new applications.
Scholaert C., Janzakova K., Coffinier Y., Pecqueur S., Alibart F.
Abstract: 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 cales 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 i ntegrates 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 no de halfway between the two realms of brain and electronic communication.
Scholaert C., Janzakova K., Coffinier Y., Alibart F., Pecqueur S.*
Abstract: During recent years, neuromorphic engineering has gained significant attraction due to its endeavor to reproduce attractive brain features such as high computational efficiency, low power consumption, functional and structural adaptability onto hardware devices for competitive computing development. Currently, most of these implementations are achieved with either standard silicon-based technologies (complementary metal-oxide-semiconductor) or more emerging material and devices (iono-electronic material s and memristor devices). Mainly, these technologies are produced by means of top-down approaches. In contrast, brain computing largely relies on self-assembling processes to interconnect cells and form pathways for neural networks communication. Thus, t o benefit more from neuromorphic features, there is a strong need to explore such devices that can rely on the same bottom-up approach as in the brain. Promising solutions for this question are gathered in organic electronic materials, more precisely in organic mixed ionic electronic conductors. This study is focused on the development of bottom-up fashioned 3D organic devices that are able to mimic biological neural network branching. By employing Alternating-Current (AC) bipolar electropolymerization, we show how one can synthesize polymer dendritic structures and tune its morphologies depending on various applied AC signals . Additionally, we show how dendritic devices may exhibit synaptic plasticity properties (short-term and long-term memory effec t). Finally, we demonstrate implementation of structural plasticity through spike-event activation AC-electropolymerization and the possibility to modify the weight of obtained dendritic connections with respect to spike rate intensity of the applied sig nals.
Janzakova K., Ghazal M., Kumar A., Coffinier Y., Pecqueur S., Alibart F.
Abstract: Over the past few years, organic electronics - and especially organic mixed ionic electronic conductors (OMIECs) - has taken bio sensing and neuromorphic applications to a whole new level. However, one of the major limitations of the mainstream technolog ies today is that electronic circuits need to be pre-shaped according to the intended use and the expected outcome. This top-down approach, far from being flexible/adaptive, does not really make the most of the resources at hand, as it is hard to predict precisely where cells will be located. To counter that, we can either choose to increase the density and the number of electrodes, so that the entire area would be mapped, or shift from a top-down to a bottom-up approach which would allow for a more enl ightened decision-making process. Recently, the electrodeposition of PEDOT:PSS has been explored as a novel technique to grow conducting polymer films and fibers on non-conductive substrates. The work of Janzakova and coworkers took that concept a step f urther by using electropolymerization of EDOT as a way to create freestanding dendritic-like conductive fibers in a 3D environment, paving the way for in operando material modification, and in fine bottom-up fabrication routes that would be more adaptive and allow for more flexibility. Moreover, it was lately showed that these objects could work as Organic Electrochemical Transistors (OECTs). Here, we explore the possibility of growing dendritic-like PEDOT fibers on Multielectrode Arrays (MEAs) via elec tropolymerization of EDOT. Electrophysiological measurements are based on the capacitive coupling between cells and the electrode material. In comparison with local electrodes, the dendritic objects present spatially distributed impedance due to the exte nsions of their dendritic branches interacting with the biological environment. We investigate the relation between morphology and impedance in these dendritic-like fibers by using a non-conventional Electrochemical Impedance Spectroscopy (EIS) setup tha t will allow us to apply a potential difference between the two ends of the dendrites, thus studying how biasing them can affect their behavior. Moreover, it appears that dendritic fibers can be considered both as passive electrodes as well as active dev ices. We explore the use of these two strategies in the context of electrophysiological measurements. Finally, the ability to record biological signals results from the interaction between cells and an electrode. Unconventional objects such as dendrites present spatio-temporal filtering properties that could affect the recording of such signals. We investigate how tuning the impedance of a dendrite might be used to record efficiently bio-signals.
Scholaert C., Janzakova K., Ghazal M., Daher Mansour M., Lefebvre C., Halliez S., Coffinier Y., Pecqueur S., Alibart F.
Abstract: Iono-electronic materials and devices are suscitating lots of interest from both bio-electronics and neuromorphic research communities. In the one hand, iono-electronic materials are offering attractive features such as bio-compatibility, water environme nt operation and efficient ionic to electronic signals transduction. In the other hand, functional devices based on such materials (organic electrochemical transistors, for instance) have shown multiple neuromorphic features from synaptic plasticity to d endritic integration. This talk will present how electropolymerization of PEDOT:PSS materials can be used in both a bio-electronic and a neuromorphic perspective. Electropolymerization of OECT sensors can indeed be advantageously used for optimizing / tu ning the iono-electronic responses of organic electrochemical transistors, thus paving the way to plastic electrophysiological sensors. Notably, we will show how transconductance and volumetric capacitance are evolving with potenstiostatic electropolymer ization. Secondly, bipolar AC electropolymerization can be used to engineer dendritic-like fibers of PEDOT:PSS. Such unconventional structures can implement various neuromorphic concept such as structural plasticity and synaptic plasticity. Finally, comp uting task taking advantage of both electropolymerized sensors and neuromorphic computing will present temporal patterns classification with reservoir computing approach.
Alibart F., Ghazal M., Janzakova K., Kumar A., Scholaert C., Coffinier Y., Pecqueur S.
Abstract: 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 whi ch 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' s hapes. 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 p henomenon 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 parti cles 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 an d 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.
Kumar A.*, Janzakova K., Coffinier Y., Pecqueur S., Alibart F.
Abstract: 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 electr opolymerization 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 degr ee, 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 imp edance 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 impleme ntation 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.
Janzakova K., Kumar A., Ghazal M., Susloparova A., Coffinier Y., Alibart F., Pecqueur S.*
Abstract: 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 re alized 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, an d structural plasticity, which are essential features required for future neuromorphic hardware development.},
Janzakova K., Ghazal M., Kumar A., Coffinier Y., Pecqueur S.*, Alibart F.*
Abstract: Most of today's strategies to interface biology with electronic hardware are based on layered architectures where the front-end of sensing is optimized separately from the back-end for processing/computing signals. Alternatively, biological systems are c apitalizing on distributed architecture where both sensing and computing are mix together and co-optimized. In this talk, we will present our strategy to implement bio-sensing of electroactive cells in a neuromorphic perspective. We will present how orga nic electrochemical transistors can be used to record electrical signals from neural cells. We will show various strategies capitalizing on the versatility of organic materials synthesis and organic device fabrication to tune and adapt the functionalitie s of such bio-sensors. We will then present how these strategies can be efficiently used to realize computing functions directly at the interface with biology. Notably, we will illustrate how a network of ionic sensors can implement the reservoir computi ng concept, a powerful neuromorphic computing approach of particular interest for dynamical signal processing.
Alibart F., Ghazal M., Janzakova K., Kumar A., Susloparova A., Halliez S., Colin M., Buée L., Guérin D., Dargent T., Coffinier Y., Pecqueur S.
Abstract: Electropolymerization is an interesting bottom-up strategy to structure conducting materials at the micro/nano-scale in liquid phase that offers a wide morphological versatility. Since the geometry of these structures governs their electrochemical proper ties, it is fundamental to decipher the mechanisms that rule the polymer assembling upon the electrically-programmed growth to use this phenomenon as a neuro-inspired building block for unconventional information processing. Herein, we investigate variou s electrical parameters of electropolymerization affecting the conducting polymer network geometry. We find that various structures such as dendrites, trees, fractals as well as low-fractality cables can be obtained between the two-wire electrodes, based on applied voltage amplitude, biasing symmetry, bias frequency, the concentration of monomers and electrode configurations. We qualitatively and quantitatively study the relationship between the electrical parameters affecting geometrical parameters of the conducting polymer network as well as electropolymerization dynamics through video and image processing. The systematic analysis shows that an increase in applied voltage leads to higher growth rate, more branches, and lower surface to bulk ratio. At the other hand, an increase in bias frequency leads to higher growth rate, smaller number of branches, and higher surface to volume ratio. In order to model the experimental phenomena, we simulate a simplified version of the problem with two bipolar met al electrodes and an electrolyte filled with dilute moving particles at random positions, reflecting the monomers in the liquid phase. The wire electrodes are biased with AC frequency and the spacio-temporal potential map is evaluated by solving the Lapl ace equation. The motion of the monomer particles is controlled by the electric field and by random Brownian motion. The particles that happen to touch the electrodes are stuck to the electrodes, with a certain probability of sticking. The stuck particle s are incorporated into the electrode, and the potential is recalculated for the motion of the particles;. The simulations are tested for different AC applied voltages, frequency, duty cycles, and voltage offsets. The increase in applied voltage leads to higher sticking probability; resulting in a higher growth rate, multiple branches, and higher density, which goes well with the experiments. Further, the effect of frequency, which is not so intuitive, shows that higher AC frequency, favors linear cable like growth, while lower frequency leads to more isotropic growth, while voltage offset and non-equal duty cycle lead to asymmetrical growth, in accordance with experiments. In addition, the effect of electrode spacing, different electrode designs, elec trical pulse shapes and the concentration of particles, are also studied. The study helps in visualizing the motion of particles in different electrical conditions, which is not possible to probe experimentally. Some subtle experimental features, such as the effect of preferential growth on the tips, and broadening of the electrode before touching, are observed in the modeling studies. Thus, we find that the different network architectures are associated with different Laplace end diffusion fields gover ning the monomers motion and in turn electropolymerized network geometry. Such unconventional engineering route could have a variety of applications from neuromorphic engineering to bottom-up computing strategies.
Kumar A., Janzakova K., Coffinier Y., Guérin D., Alibart F., Pecqueur S.
Abstract: Most of today's strategies to interface biology with electronic hardware are based on layered architectures where the front-end of sensing is optimized separately from the back-end for processing/computing signals. Alternatively, biological systems are c apitalizing on distributed architecture where both sensing and computing are mix together and co-optimized. In this talk, we will present our strategy to implement bio-sensing of electroactive cells in a neuromorphic perspective. We will present how orga nic electrochemical transistors can be used to record electrical signals from neural cells. We will show various strategies capitalizing on the versatility of organic materials synthesis and organic device fabrication to tune and adapt the functionalitie s of such bio-sensors. We will then present how these strategies can be efficiently used to realize computing functions directly at the interface with biology. Notably, we will illustrate how a network of ionic sensors can implement the reservoir computi ng concept, a powerful neuromorphic computing approach of particular interest for dynamical signal processing.
Alibart F., Ghazal M., Janzakova K., Kumar A., Susloparova A., Halliez S., Colin M., Buée L., Guérin D., Dargent T., Coffinier Y., Pecqueur S.
Abstract: One of the neuromorphic engineering aims is using nanoelectronics' materials and devices to reproduce key features that are used by the brain for computing. Currently, neuromorphic engineering has explored standard silicon-based technologies (i.e. such a s complementary metal-oxide-semiconductor ) or more emerging material and devices (iono-electronic materials and resistive memory devices, for example). Most of these technologies are still bounded to a top down approach. However, brain computing largely rely on bottom-up processes. For instance, interconnectivity between cells and formation of communication pathway in neural networks result principaly from bottom-up organization. Here, we show how dendritic growth of organic conductive polymers (PEDOT) can be used to mimic structural branching observed in neural network. Conducting-polymer based dendritic structures with different morphology are synthesized in a two-electrode setup by pulsed voltage-driven electropolymerization derived from state-of-t he-art bipolar AC-electrochemical synthetic methods. We show how various AC signals can lead to a large variety of dendritic structures and PEDOT morphologies. In a second part, such dendritic structures are used to implement functionnal OECTs. More impo rtantly, we focus on the transconductance and memory effects that can be obtained in such dendritic OECTs such as short tem plasticity. We report on the relationship between dendrites morphologies and STP time constant. This work paves the way to new app roaches for neuromorphic engineering, such as structural plasticity and neural network topology exploration.
Janzakova K., Ghazal M., Kumar A., Coffinier Y., Guérin D., Pecqueur S., Alibart F.
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