Becker, MaximilianLoche, Philip RobinRezaei, MajidWolde-Kidan, AmanuelUematsu, YukiNetz, Roland R.Bonthuis, Douwe Jan2024-02-232024-02-232024-02-232023-12-2010.1021/acs.chemrev.3c00307https://infoscience.epfl.ch/handle/20.500.14299/205280WOS:001140846800001From the stability of colloidal suspensions to the charging of electrodes, electric double layers play a pivotal role in aqueous systems. The interactions between interfaces, water molecules, ions and other solutes making up the electrical double layer span length scales from & Aring;ngstroms to micrometers and are notoriously complex. Therefore, explaining experimental observations in terms of the double layer's molecular structure has been a long-standing challenge in physical chemistry, yet recent advances in simulations techniques and computational power have led to tremendous progress. In particular, the past decades have seen the development of a multiscale theoretical framework based on the combination of quantum density functional theory, force-field based simulations and continuum theory. In this Review, we discuss these theoretical developments and make quantitative comparisons to experimental results from, among other techniques, sum-frequency generation, atomic-force microscopy, and electrokinetics. Starting from the vapor/water interface, we treat a range of qualitatively different types of surfaces, varying from soft to solid, from hydrophilic to hydrophobic, and from charged to uncharged.Physical SciencesLiquid-Vapor InterfaceWater-MoleculesSurface-TensionIon SolvationFree-EnergyHydrophilic SurfacesDielectric-ConstantPolar FluidsForce-FieldFrequencytext::journal::journal article::review article