Electroferrofluids with non-equilibrium voltage-controlled magnetism, interfaces, and patterns

Abstract

Materials with continuous dissipation can exhibit responses and functionalities that are not possible in thermodynamic equilibrium. While this concept is well-known, a major challenge has been the implementation: how to rationally design materials with functional non-equilibrium states and quantify the dissipation? Here we address these questions for the widely used colloidal nanoparticles that convey several functionalities. We propose that useful non-equilibrium states can be realised by creating and maintaining steady-state nanoparticle concentration gradients by continuous injection and dissipation of energy. We experimentally demonstrate this with superparamagnetic iron oxide nanoparticles that in thermodynamic equilibrium form a homogeneous functional fluid with a strong magnetic response (a ferrofluid). To create non-equilibrium functionalities, we charge the nanoparticles with anionic charge control agents to create electroferrofluids where nanoparticles act as charge carriers that can be driven with electric fields and current to non-homogeneous dissipative steady-states. The dissipative steady-states exhibit voltage-controlled magnetic properties and emergent diffuse interfaces. The diffuse interfaces respond strongly to external magnetic fields, leading to dissipative patterns that are not possible in the equilibrium state. We identify the closest non-dissipative analogues of these dissipative patterns, discuss the differences, and highlight how pattern formation in electroferrofluids is linked to dissipation that can be directly quantified. Beyond electrically controlled ferrofluids and patterns, we foresee that the concept can be generalized to other functional nanoparticles to create various scientifically and technologically relevant non-equilibrium states with optical, electrical, catalytic, and mechanical responses that are not possible in thermodynamic equilibrium.