10.1021/acsomega.8b01393.s001 Inderbir S. Sidhu Inderbir S. Sidhu Amalie L. Frischknecht Amalie L. Frischknecht Paul J. Atzberger Paul J. Atzberger Electrostatics of Nanoparticle–Wall Interactions within Nanochannels: Role of Double-Layer Structure and Ion–Ion Correlations American Chemical Society 2018 ion effects channel walls energy barriers Double-Layer Structure coarse-grained particle-level simulations nanoparticle locations Brownian dynamics investigation free-energy profile like-charged nanoparticles nanoscale devices electrolyte strength electrolyte-mediated interactions charge regimes energy minima 2018-09-18 18:33:56 Journal contribution https://acs.figshare.com/articles/journal_contribution/Electrostatics_of_Nanoparticle_Wall_Interactions_within_Nanochannels_Role_of_Double-Layer_Structure_and_Ion_Ion_Correlations/7100522 We perform computational investigations of the electrolyte-mediated interactions of charged nanoparticles with the walls of nanochannels. We investigate the role of discrete ion effects, valence, and electrolyte strength on nanoparticle–wall interactions. We find for some of the multivalent charge regimes that the like-charged nanoparticles and walls can have attractive interactions. We study in detail these interactions and the free-energy profile for the nanoparticle–wall separation. We find there are energy barriers and energy minima giving preferred nanoparticle locations in the channel near the center and at a distance near to but separated from the channel walls. We characterize contributions from surface overcharging, condensed layers, and overlap of ion double layers. We perform our investigations using coarse-grained particle-level simulations with Brownian dynamics, classical density functional theory, and the mean-field Poisson–Boltzmann theory. We discuss the implications of our results for phenomena in nanoscale devices.