A Mode-Coupling Model of Colloid Thermophoresis in Aqueous Systems: Temperature and Size Dependencies of the Soret Coefficient.

Thermophoresis allows for the manipulation of colloids in systems containing a temperature gradient. A deep understanding of the phenomena at the molecular level allows for increased control and manipulation strategies. We developed a microscopic model revealing different coupling mechanisms for colloid thermophoresis under local thermodynamic equilibrium conditions. The model has been verified through comparison with a variety of previously published experimental data and shows good agreement across significantly different systems. We found five different temperature-dependent contributions to the Soret coefficient, two from bulk properties and three from interfacial interactions between the fluid medium and the colloid. Our analysis shows that the Soret coefficient for nanosized particles is governed by the competition between the electrostatic and hydration interfacial interactions, while bulk contributions become more pronounced for protein systems. This theory can be used as a guide to design thermophoretic transport, which is relevant for sensing, focusing, and separation at the microscale.