What controls thermo-osmosis? Molecular simulations show the critical role of interfacial hydrodynamics

Abstract

Thermo-osmotic and related thermo-phoretic phenomena can be found in many situations from biology to colloid science, but the underlying molecular mechanisms remain largely unexplored. Using molecular dynamics simulations, we measured the thermo-osmosis coefficient by both mechano-caloric and thermo-osmotic routes, for different solid-liquid interfacial energies. The simulations reveal in particular the crucial role of nanoscale interfacial hydrodynamics. For non-wetting surfaces , thermo-osmotic transport is largely amplified by hydrodynamic slip at the interface. For wetting surfaces, the position of the hydrodynamic shear plane plays a key role in determining the amplitude and sign of the thermo-osmosis coefficient. Finally, we measure a giant thermo-osmotic response of the water-graphene interface, which we relate to the very low interfacial friction displayed by this system. These results open new perspectives for the design of efficient functional interfaces for, e.g., waste heat harvesting.