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Abstract We performed numerical simulations with the Kuramoto model and experiments with oscillatory nickel electrodissolution to explore the dynamical features of the transients from random initial conditions to a fully synchronized (one-cluster) state. The numerical simulations revealed that certain networks (e.g., globally coupled or dense Erdős–Rényi random networks) showed relatively simple behavior with monotonic increase of the Kuramoto order parameter from the random initial condition to the fully synchronized state and that the transient times exhibited a unimodal distribution. However, some modular networks with bridge elements were identified which exhibited non-monotonic variation of the order parameter with local maximum and/or minimum. In these networks, the histogram of the transients times became bimodal and the mean transient time scaled well with inverse of the magnitude of the second largest eigenvalue of the network Laplacian matrix. The non-monotonic transients increase the relative standard deviations from about 0.3 to 0.5, i.e., the transient times became more diverse. The non-monotonic transients are related to generation of phase patterns where the modules are synchronized but approximately anti-phase to each other. The predictions of the numerical simulations were demonstrated in a population of coupled oscillatory electrochemical reactions in global, modular, and irregular tree networks. The findings clarify the role of network structure in generation of complex transients that can, for example, play a role in intermittent desynchronization of the circadian clock due to external cues or in deep brain stimulations where long transients are required after a desynchronization stimulus. 

Coupled oscillator networks often display transitions between qualitatively different phase-locked solutions—such as synchrony and rotating wave solutions—following perturbation or parameter variation. In the limit of weak coupling, these transitions can be understood in terms of commonly studied phase approximations. As the coupling strength increases, however, predicting the location and criticality of transition, whether continuous or discontinuous, from the phase dynamics may depend on the order of the phase approximation—or a phase description of the network dynamics that neglects amplitudes may become impossible altogether. Here we analyze synchronization transitions and their criticality systematically for varying coupling strength in theory and experiments with coupled electrochemical oscillators. First, we analyze bifurcations analysis of synchrony and splay states in an abstract phase model and discuss conditions under which synchronization transitions with different criticalities are possible. In particular, we show that such conditions can be understood by considering the relative contributions of higher harmonics to the phase dynamics. Second, we illustrate that transitions with different criticality indeed occur in experimental systems. Third, we highlight that the amplitude dynamics observed in the experiments can be captured in a numerical bifurcation analysis of delay-coupled oscillators. Our results showcase that reduced order phase models may miss important features that one would expect in the dynamics of the full system. Published by the American Physical Society2024 

We investigate the entrainment of electrochemical oscillators with different phase response curves (PRCs) using a global signal: the goal is to achieve the desired phase configuration using a minimum-power waveform. Establishing the desired phase relationships in a highly nonlinear networked system exhibiting significant heterogeneities, such as different conditions or parameters for the oscillators, presents a considerable challenge because different units respond differently to the common global entraining signal. In this work, we apply an optimal phase-selective entrainment technique in both a kinetic model and experiments involving electrochemical oscillators in achieving phase synchronized states. We estimate the PRCs of the oscillators at different circuit potentials and external resistance, and entrain pairs and small sets of four oscillators in various phase configurations. We show that for small PRC variations, phase assignment can be achieved using an averaged PRC in the control design. However, when the PRCs are sufficiently different, individual PRCs are needed to entrain the system with the expected phase relationships. The results show that oscillator assemblies with heterogeneous PRCs can be effectively entrained to desired phase configurations in practical settings. These findings open new avenues to applications in biological and engineered oscillator systems where synchronization patterns are essential for system performance. 

We investigate the dynamical behavior of the oscillatory electrodissolution of nickel and hydrogen reduction reaction in a closed electrochemical bipolar cell with two nickel wires. In the bipolar setup, two-half U cells are separated by an epoxy plate with the two embedded nickel electrodes; the oxidation and reduction reactions take place at the two ends of the same wire. The electrode potential oscillations were found to be strongly synchronized with 1 mm diameter electrodes in an in-phase configuration. Because experiments in similar configurations with traditional (three-electrode) cell showed no synchronization of the oscillatory anodic nickel electrodissolution, the introduction of the cathodic side of the bipolar electrodes induced the synchronization. The results were interpreted with a model that considered the kinetically coupled cathode-anode dynamics as well as interactions on the cathode and the anode side through migration current mediated potential drops in the electrolyte. The electrical coupling strength was calculated from solution resistance and charge transfer resistance measurements. The theory correctly interpreted that the bipolar cell with large (1 mm diameter) electrodes exhibits strong coupling with synchronization, and the bipolar cell with small (0.25 mm diameter) electrodes and the traditional configuration exhibit weak coupling and thus desynchronization. The experiments demonstrate the use of bipolar electrochemical cells for the investigation of collective behavior of electrochemical processes and the proposed approach holds promise for the design of bipolar multi-electrode arrays with engineered coupling to promote sensing and information processing using microchips. 

We investigate the emergence of current oscillations of a bipolar electrode (BPE) in coupled anode/cathode reaction under potentiostatic condition. In a traditional three-electrode setup, the nickel dissolution in sulfuric acid requires a minimum amount of IR ohmic drop, and thus series resistance for the oscillations to occur. In this paper, it is shown that in bipolar setup, when the nickel electrodissolution on the anodic side is coupled to hydrogen ion reduction on the cathodic side, spontaneous current oscillations can occur. An electrochemical analysis of the dynamics shows that the required circuit potential for the oscillations can be predicted from estimating the overpotentials needed for the anodic and cathodic reactions, the driving electrode, and the ohmic drop in the electrolyte. The dynamics and range of oscillations can be tuned by different concentrations of electrolyte, on both the anodic and the cathodic sides. In the considered example, the charge transfer resistance of the cathodic reaction can provide sufficient total resistance even when the solution resistance does not yield sufficient IR drop for the oscillations. Our findings have the potential to promote further studies of the collective behavior of electrochemical reactions using multielectrode arrays in bipolar electrode setups. 

The spatiotemporal organization of networks of dynamical units can break down resulting in diseases (e.g., in the brain) or large-scale malfunctions (e.g., power grid blackouts). Re-establishment of function then requires identification of the optimal intervention site from which the network behavior is most efficiently re-stabilized. Here, we consider one such scenario with a network of units with oscillatory dynamics, which can be suppressed by sufficiently strong coupling and stabilizing a single unit, i.e., pinning control. We analyze the stability of the network with hyperbolas in the control gain vs coupling strength state space and identify the most influential node (MIN) as the node that requires the weakest coupling to stabilize the network in the limit of very strong control gain. A computationally efficient method, based on the Moore–Penrose pseudoinverse of the network Laplacian matrix, was found to be efficient in identifying the MIN. In addition, we have found that in some networks, the MIN relocates when the control gain is changed, and thus, different nodes are the most influential ones for weakly and strongly coupled networks. A control theoretic measure is proposed to identify networks with unique or relocating MINs. We have identified real-world networks with relocating MINs, such as social and power grid networks. The results were confirmed in experiments with networks of chemical reactions, where oscillations in the networks were effectively suppressed through the pinning of a single reaction site determined by the computational method. 

The synchronization dynamics for the circadian gene expression in the suprachiasmatic nucleus is investigated using a transcriptional circadian clock gene oscillator model. With global coupling in constant dark (DD) conditions, the model exhibits a one-cluster phase synchronized state, in dim light (dim LL), bistability between one- and two-cluster states and in bright LL, a two-cluster state. The two-cluster phase synchronized state, where some oscillator pairs synchronize in-phase, and some anti-phase, can explain the splitting of the circadian clock, i.e., generation of two bouts of daily activities with certain species, e.g., with hamsters. The one- and two-cluster states can be reached by transferring the animal from DD or bright LL to dim LL, i.e., the circadian synchrony has a memory effect. The stability of the one- and two-cluster states was interpreted analytically by extracting phase models from the ordinary differential equation models. In a modular network with two strongly coupled oscillator populations with weak intragroup coupling, with appropriate initial conditions, one group is synchronized to the one-cluster state and the other group to the two-cluster state, resulting in a weak-chimera state. Computational modeling suggests that the daily rhythms in sleep–wake depend on light intensity acting on bilateral networks of suprachiasmatic nucleus (SCN) oscillators. Addition of a network heterogeneity (coupling between the left and right SCN) allowed the system to exhibit chimera states. The simulations can guide experiments in the circadian rhythm research to explore the effect of light intensity on the complexities of circadian desynchronization. 

Abstract Networks of weakly coupled oscillators had a profound impact on our understanding of complex systems. Studies on model reconstruction from data have shown prevalent contributions from hypernetworks with triplet and higher interactions among oscillators, in spite that such models were originally defined as oscillator networks with pairwise interactions. Here, we show that hypernetworks can spontaneously emerge even in the presence of pairwise albeit nonlinear coupling given certain triplet frequency resonance conditions. The results are demonstrated in experiments with electrochemical oscillators and in simulations with integrate-and-fire neurons. By developing a comprehensive theory, we uncover the mechanism for emergent hypernetworks by identifying appearing and forbidden frequency resonant conditions. Furthermore, it is shown that microscopic linear (difference) coupling among units results in coupled mean fields, which have sufficient nonlinearity to facilitate hypernetworks. Our findings shed light on the apparent abundance of hypernetworks and provide a constructive way to predict and engineer their emergence. 

A passive electrochemical coupling approach is proposed to induce spontaneous synchronization between chemical oscillators. The coupling exploits the potential difference between a catalyst redox couple in the Belousov–Zhabotinsky (BZ) reaction, without external feedback, to induce surface reactions that impact the kinetics of the bulk system. The effect of coupling in BZ oscillators under batch condition is characterized using phase synchronization measures. Although the frequency of the oscillators decreases nonlinearly over time, by a factor of 2 or more within 100 cycles, the coupling is strong enough to maintain synchronization. In such a highly drifting system, the Gibbs–Shannon entropy of the cyclic phase difference distribution can be used to quantify the coupling effect. We extend the Oregonator BZ model to account for the drifting natural frequencies in batch condition and for electrochemical coupling, and numerical simulations of the effect of acid concentration on synchronization patterns are in agreement with the experiments. Because of the passive nature of coupling, the proposed coupling scheme can open avenues for designing pattern recognition and neuromorphic computation systems using chemical reactions in a spontaneous process.