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Microparticles migrate in response to gradients in solute concentrationthrough diffusiophoresis and diffusioosmosis. Merging streams of fluid withdistinct solute concentrations is a common strategy for producing a steadyconcentration gradient with continuous flow in microfluidic devices; the soluteconcentration gradient and consequent diffusiophoresis are primarily normal tothe background flow. This is particularly useful in separation and filtrationprocesses, as it results in regions of particle accrual and depletion incontinuous flows. Such systems have been examined in several classic papers ondiffusiophoresis, with a focus on the particle dynamics far from boundaries. Weshow, through experiments, simulations, and theory, that diffusioosmotic flowalong certain boundaries can result in significant changes in particle dynamicsand particle focusing in near-wall regions. The nonzero velocity at chargedsurfaces draws solute and particles along the boundary until the flowultimately recirculates. These "convection rolls," which result in the spanwisemigration of polystyrene particles close to boundaries, are apparent near aglass surface but vanish when the surface is coated with gold. Thethree-dimensional nature of the dynamics could have implications for the designof microfluidic devices: Channel materials can be selected to enhance orsuppress near-wall flows. Additionally, we demonstrate the importance ofconsidering solute concentration-dependent models for diffusiophoretic anddiffusioosmotic mobility in capturing the dynamics of particles, particularlyin regions of low solute concentration.

Convection rolls and three-dimensional particle dynamics in merging solute streams