Nonlinear Thermophoresis beyond Local Equilibrium Criterion

Thermophoresis (thermodiffusion, Soret effect) moves molecules along thermal gradients. We measure its phenomenological linear drift relation by single particle tracking in convection-free settings. For moderate thermal gradients, drift velocity depends linearly on the gradient. However, for strong thermal gradients, we find a nonlinear dependence of the drift on the applied gradient for large Soret coefficient and particle radius. Interestingly, the onset of the nonlinearity coincides with a local disequilibrium of the particle. Nonlinear thermophoresis resolves several fundamental contradictions between thermophoretic experiments and theory.