At the interface between an electrode and electrolyte the electric double layer (EDL), featuring a considerably large potential change within a few Ångströms and a complex interplay of charges between solvent dipoles, charged adsorbates and the diffuse ion layer, is formed. Deepened understanding of the EDL is a stringent necessity for the knowledge-based advancement of electrochemical processes occurring in technologically relevant settings such as energy conversion, storage devices and solar cells. Despite its high significance, a complete and comprehensive atomic-level description of the EDL including interfacial structures and dynamics is so far lacking. Here, its complexity and difficulty to probe have been challenged in recent years both experimentally (e.g. via X-ray photoelectron spectroscopy (XPS), Raman spectroscopy, laser-induced temperature jump methods, 7 cyclic voltammetry (CV) or sum frequency generation spectroscopy 9 ) and theoretically via empirical interatomic force field simulations and first-principles calculations (e.g. ab initio molecular dynamics (AIMD), 10,11 see also ref. 12,13 and references therein).