Nonlinearities in shadowgraphy experiments on non-equilibrium fluctuations in polymer solutions

Giant thermal and solutal non-equilibrium fluctuations are observed in shadowgraphy experiments on liquid mixtures subjected to a temperature gradient. For large temperature differences, both the temperature and the composition dependence of the relevant thermophysical parameters and the nonlinear terms in the diffusion equation need to be taken into account, leading to a nonlinear concentration profile. For temperature differences exceeding the inverse of the Soret coefficient, in our example approximately 10 K, the usual data evaluation yields increasingly wrong diffusion and Soret coefficients that are off by almost a factor of two for a temperature difference of 50 K. A local model that treats the measured shadowgraph signal as a superposition of the contributions from every layer of the sample is able to capture the essential trend and yields a good agreement with experimental data. The results are important for the application of shadowgraphy as a tool for the measurement of Soret and diffusion coefficients, where large temperature gradients promise a good signal-to-noise ratio.