Forced Crowding of Colloids by Thermophoresis and Convection in a Custom Liquid Clusius-Dickel Microdevice.

We report a study demonstrating that simultaneous induction of a steady-state convection current and temperature gradient in a confined geometry can be an effective way to force crowding of dissolved particulates. To investigate this thermogravitationally driven concentration of particles in situ, we developed a microdevice capable of sustaining controlled transverse temperature gradients within a 5 cm long, 0.1 mm inner diameter capillary that allowed visualization of particle movement with standard optical microscopy. Experiments were conducted on two material systems representative of nanoscale small molecules and microscale particles. With the small molecules (aromatic dyes, 530-790 g/mol, 1-1.5 nm), thermophoretic and gravitational effects in the microdevice resulted in an asymmetrical 2× concentration change along the capillary height over 3 days. In contrast, the concentration change under similar conditions for 40-micron diameter latex colloids is 50-fold in 30 min. This dramatic difference in separation times is consistent with simulations and models of thermophoresis where the thermophoretic effect scales with particle size. Induced crowding of particulates leads to formation of accumulation and depletion zones at the bottom and top of the capillary, respectively. Both the concentration of dye molecules over time in the depletion zone and the spatial distribution of colloids over the entire capillary length were found to be good fits to simple first-order exponential decay functions. These results suggest potential applications of thermogravitational separation in developing new functional materials via thermophoretic and convective effects.