Direct evidence is provided for the transition from surface conduction (SC) to electro-osmotic flow (EOF) above a critical channel depth (d) of a nanofluidic device. The dependence of the overlimiting conductance (OLC) on d is consistent with theoretical predictions, scaling as d −1 for SC and d 4=5 for EOF with a minimum around d ¼ 8 μm. The propagation of transient deionization shocks is also visualized, revealing complex patterns of EOF vortices and unstable convection with increasing d. This unified picture of surface-driven OLC can guide further advances in electrokinetic theory, as well as engineering applications of ion concentration polarization in microfluidics and porous media.

Recently, tremendous engineering applications utilizing new physics of nanoscale electrokinetics have been reported and their basic fundamentals are actively researched. In this work, we first report a simple and economic but reliable nanochannel fabrication technique, leading to a heterogeneously charged triangular nanochannel. The nanochannel utilized the elasticity of PDMS when it bonded with a micrometer-scale structure on a substrate. Second, we successfully demonstrated novel ionic transportations by tweaking the micrometer structures: (1) the transition of nonlinear ionic conductance depending on the nanochannel properties and (2) the ionic field-effect transistor. Nanochannel conductance has two distinguishable nonlinear regimes called the "surface-charge-governed" and the "geometry-governed" regime and its only individual overlooks were frequently reported. However, the transition between two regimes by adjusting nanochannel properties has not been reported due to the difficulty of functional nanochannel fabrication. In addition, a gate voltage was comfortably applied to the triangular nanochannel so that the field-effect ion transportation was reliably achieved. Therefore, presenting triangular nanochannels have critical advantages over its heterogeneous and tunable surface properties and thus, could be an effective means as an active fundamental to control and manipulate the ion-electromigration through a nanofluidic system.

Nanofabrication technologies have been a strong advocator for new scientific fundamentals that have never been described by traditional theory, and have played a seed role in ground-breaking nanoengineering applications. In this study, we fabricated ultra-high-aspect ($10 6 with O(100) nm nanochannel opening and O(100) mm length) orthogonal nanochannel array using only polymeric materials. Vertically aligned nanochannel arrays in parallel can be stacked to form a dense nanostructure. Due to the flexibility and stretchability of the material, one can tune the size and shape of the nanochannel using elongation and even roll the stack array to form a radial-uniformly distributed nanochannel array. The roll can be cut at discretionary lengths for incorporation with a micro/ nanofluidic device. As examples, we demonstrated ion concentration polarization with the device for Ohmic-limiting/overlimiting current-voltage characteristics and preconcentrated charged species. The density of the nanochannel array was lower than conventional nanoporous membranes, such as anodic aluminum oxide membranes (AAO). However, accurate controllability over the nanochannel array dimensions enabled multiplexed one microstructure-on-one nanostructure interfacing for valuable biological/biomedical microelectromechanical system (BioMEMS) platforms, such as nanoelectroporation.

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