A dynamically equivalent atomistic electrochemical paradigm for the larger-scale experiments

Abstract

Electrochemical systems possess a considerable part of modern technologies, such as the operation of rechargeable batteries and the fabrication of electronic components, which are explored both experimentally and computationally. The largest gap between the experimental observations and atomic-level simulations is their orders-of-magnitude scale difference. While the largest computationally affordable scale of the atomic-level computations is ∼ns and ∼nm, the smallest reachable scale in the typical experiments, using very high-precision devices, is ∼s and ∼μm. In order to close this gap and correlate the studies in the two scales, we establish an equivalent simulation setup for the given general experiment, which excludes the microstructure effects (i.e., solid–electrolyte interface), using the coarse-grained framework. The developed equivalent paradigm constitutes the adjusted values for the equivalent length scale (i.e., lEQ), diffusivity (i.e., DEQ), and voltage (i.e., VEQ). The time scale for the formation and relaxation of the concentration gradients in the vicinity of the electrode matches for both smaller scale (i.e., atomistic) equivalent simulations and the larger scale (i.e., continuum) experiments and could be utilized for exploring the cluster-level inter-ionic events that occur during the extended time periods. The developed model could offer insights for forecasting experiment dynamics and estimating the transition period to the steady-state regime of operation.