Prediction of the Initial stages of electrochemical phase formation by multi-scale modelling and in-situ transmission electron microscopy

Electrodeposition offers the most versatile and scalable route formaterial growth. However, our current understanding is inaccurateand incomplete: electrochemical nucleation and growth (EN&G) doesnot proceed only by a classical pathway (direct attachment of ionsfrom solution), but also by non-classical routes (nanocluster surfacediffusion & aggregation, etc.).Our goal is to develop a comprehensive model to predict the initialstages of electrochemical phase formation taking non-classicalgrowth pathways into account.To get consistent experimental data on nucleation and growthkinetics, an in-situ method with high resolution is essential. For this,in-situ electrochemical transmission electron microscopy (EC-TEM) isbest suited since it allows recording videos where nanometer-sizedfeatures are visualized dynamically.Yet, the method has important limitations: accelerated electronsinteract with the electrodes and species in solution, altering theEN&G kinetics and preventing a correct interpretation of EC-TEMdata. Although the electron beam effects can be partially mitigated,they cannot be completely avoided.To solve this, we propose a combined modelling-experimental approach to (1) optimize the experimental conditions so the influenceof the electron beam in EN&G is minimized; and(2) model theunavoidable effect of electron beam irradiation in electrochemical, solution and surface processes so kinetic data on EN&G can becorrectly interpreted.