Abstract: Extracting relevant data from real-world experiments is often challenging with intrinsic materials and device property dispersion, such as in organic electronics. However, multivariate data analy-sis can often be a mean to circumvent this and to extract more information when larger datasets are used with learning algorithms instead of physical models. Here, we report on identifying rele-vant information descriptors for organic electrochemical transistors (OECTs) to classify aqueous electrolytes by ionic composition. Applying periodical gate pulses at different voltage magnitudes, we extracted a reduced number of nonredundant descriptors from the rich drain-current dynam-ics, which provide enough information to cluster electrochemical data by principal component analysis between Ca2+-, K+-, and Na+-rich electrolytes. With six current values obtained at the ap-propriate time domain of the device charge/discharge transient, one can identify the cationic iden-tity of a locally probed transient current wit h only a single micrometric device. Applied to OECT-based neural sensors, this analysis demonstrates the capability for a single nonselective de-vice to retrieve the rich ionic identity of neural activity at the scale of each neuron individually when lea rning algorithms are applied to the device physics.
Pecqueur S.*, Vuillaume D., Crljen Ž., Lončarić I., Zlatić V.*
Abstract: Organic electrochemical transistors (OECTs) offer a powerful functionality for both sensing and neuro-inspired electronics with still much to understand on their time-dependent behavior. OECTs based on PEDOT:PSS conducting polymer h ave revealed two distinctive operation regimes of a device: a low frequency and a higher frequency regimes dominated by the conductance of the polymer and of the gating electrolyte, respectively. However, the systematically observed non-idealities in t he impedance spectra over the large frequency range and ionic concentrations caused by both the materials and the device complexity cannot be explained by simple models. We report on modeling of OECTs by an optimized equivalent circuit model that takes into account the frequency dependence of the device impedance from 1 Hz to 1 MHz for a large ionic concentration range (10-4 - 1 M) and various chemical nature of the ions. Based on experimental data for KCl(aq) and CaCl2(aq). the model explains the time dependency of the OECT as a whole and discusses the sensibility of new introduced elements pseudo-capacitance and inductance to concentration and voltage to understand the local physics. In particular, the observed concentrat ion-dependent negative phase change in the impedance suggests an inductive contribution to the device impedance due to the doping/dedoping process in the organic layer driven by the applied harmonic voltage as an underlying mechanism . The introduction of these non-redundant elements and the study of their behaviors as function of ionic concentration and applied voltage give a more detailed picture of the OECT working principles at a specific time domains which are highly relevant for multi-parametric ion sensing and neuromorphic computing.
Pecqueur S., Lončarić I., Zlatić V., Vuillaume D., Crljen Ž.
Abstract: Organic electrochemical transistors offer powerful functionalities for biosensors and neuro-inspired electronics, with still much to understand on the time-dependent behavior of this electrochemical device. Here, we report on distributed-element modeling of the impedance of such micro-fabricated device, systematically performed under a large concentration variation for KCl(aq) and CaCl2(aq). We propose a new model which takes into account three main deviations to ideality, that wer e systematically observed, caused by both the materials and the device complexity, over large frequency range (1 Hz-1 MHz). More than introducing more freedom degree, the introduction of these non-redundant parameters and the study of their behaviors as function of the electrolyte concentration and applied voltage give a more detailed picture of the OECT working principles. This optimized model can be further useful for improving OECT performances in many applications (e.g. biosensors, neuro-inspired de vices, ...) and circuit simulations.
Pecqueur S.*, Lončarić I., Zlatić V., Vuillaume D., Crljen Ž.*
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