All-atom molecular dynamics simulations of polymer and polyelectrolyte brushes

Densely grafted polymer and polyelectrolyte (PE) brushes, owing to their significant abilities to functionalize surfaces for a plethora of applications in sensing, diagnostics, current rectification, surface wettability modification, drug delivery, and oil recovery, have attracted significant attention over the past several decades. Unfortunately, most of the attention has primarily focused on understanding the properties of the grafted polymer and the PE chains with little attention devoted to studying the behavior of the brush-supported ions (counterions needed to screen the PE chains) and water molecules. Over the past few years, our group has been at the forefront of addressing this gap: we have employed all-atom molecular dynamics (MD) simulations for studying a wide variety of polymer and PE brush systems with specific attention to unraveling the properties and behavior of the brush-supported water molecules and ions. Our findings have revealed some of the most fascinating properties of such brush-supported ions and water molecules, including the most remarkable control of nanofluidic transport afforded by the specific ion and water responses induced by the PE brushes grafted on the inner walls of the nanochannel. This feature article aims to summarize some of our key contributions associated with such atomistic simulations of polymer and PE brushes and brush-supported water molecules and counterions. New discoveries on polymer and polyelectrolyte brush systems and the corresponding brush-supported ions and water, arising from employing all-atom molecular dynamics simulations, have been thoroughly reviewed.