Challenges in the Theory and Atomistic Simulation of Metal Electrodeposition

Electrodeposition is a fundamental process in electrochemistry and has applications in numerous industries, such as corrosion protection, decorative finishing, energy storage, catalysis, and electronics. While there is a long history of electrodeposition use, its application for controlled nanostructure growth is limited. The establishment of an atomic-scale understanding of the electrodeposition process and dynamics is crucial to enable the controlled fabrication of metal nanoparticles and other nanostructures. Significant advancements in molecular simulation capabilities and the electronic structure theory of electrified solid-liquid interfaces bring theory closer to realistic applications, but a gap remains between applications, a theoretical understanding of dynamics, and atomistic simulation. In this Review, we briefly summarize the current state-of-the-art computational techniques available for the simulation of electrodeposition and electrochemical growth on surfaces and identify the remaining open challenges.