Nanoconfinement-Enforced Ion Correlation and Nanofluidic Ion Machinery.

Machines operating at the atomic level are of fundamental interests for information manipulation and communication. However, preparation of thermodynamically stable states and regulation of transitions between them at a low energy cost are challenging. We report that, by enforcing nanoconfinement and surface gating, one can control the configurations and dynamics of ions for computational tasks. The layered structures of water confined in nanochannels render the spatial and temporal correlation between ions, offering a number of distinct states with paired configurations. Free energy barriers for transitions between them are on the order of kBT, allowing modulation through external fields or surface charges at a low energy cost. Ionic switches, rectifiers, and logical gates are constructed following the physical rules elucidated at the molecular level, opening an avenue toward artificial nanofluidic functionalities such as efficient ionic machinery by configuring the ionic pairs and controlled mass/charge transport by tuning the strength of correlation.