Determination of transport properties of fluids by optical methods

In this workshop we will discuss some fundamentals of equilibrium and non-equilibrium thermodynamics, in particular how concentration gradients are formed due to the Soret effect. At first we will pay attention to the analysis of fluctuations at macroscopic thermodynamic equilibrium for the determination of the Fick diffusion coefficient and the thermal diffusivity. Then, starting with the extended diffusion equation, we will derive solutions for the concentration field under common experimental geometries and introduce modern optical techniques for the measurement of the Fick diffusion, thermodiffusion and Soret coefficients

Slowing-down of non-equilibrium concentration fluctuations in confinement

Fluctuations in a fluid are strongly affected by the presence of a macroscopic gradient making them long-ranged and enhancing their amplitude. While small-scale fluctuations exhibit diffusive lifetimes, larger-scale fluctuations live shorter because of gravity, as theoretically and experimentally well-known. We explore here fluctuations of even larger size, comparable to the extent of the system in the direction of the gradient, and find experimental evidence of a dramatic slowing-down in their dynamics. We recover diffusive behaviour for these strongly-confined fluctuations, but with a diffusion coefficient that depends on the solutal Rayleigh number. Results from dynamic shadowgraph experiments are complemented by theoretical calculations and numerical simulations based on fluctuating hydrodynamics, and excellent agreement is found. The study of the dynamics of non-equilibrium fluctuations allows to probe and measure the competition of physical processes such as diffusion, buoyancy and confinement.Comment: Includes see Supplementary Material. Submitted to PR

Confinement effect on the dynamics of non-equilibrium concentration fluctuations far from the onset of convection

In a recent letter (C. Giraudet et al., EPL 111, 60013 (2015)) we reported preliminary data showing evidence of a slowing-down of non-equilibrium fluctuations of the concentration in thermodiffusion experiments on a binary mixture of miscible fluids. The reason for this slowing-down was attributed to the effect of confinement. Such tentative explanation is here experimentally corroborated by new measurements and theoretically substantiated by studying analytically and numerically the relevant fluctuating hydrodynamics equations. In the new experiments presented here, the magnitude of the temperature gradient is changed, confirming that the system is controlled solely by the solutal Rayleigh number, and that the slowing-down is dominated by a combined effect of the driving force of buoyancy, the dissipating force of diffusion and the confinement provided by the vertical extension of the sample cell. Moreover, a compact phenomenological interpolating formula is proposed for easy analysis of experimental results

Translational and rotational diffusion coefficients in nanofluids from polarized dynamic light scattering

Nanofluids representing nanometer-sized solid particles dispersed in liquids are of interest in many fields of process and energy engineering, e.g., heat transfer, catalysis, and the design of functionalized materials [1]. The physical, chemical, optical, and electronic properties of nanofluids are strongly driven by the size, shape, surface potential, and concentration of the nanoparticles. For the analysis of diffusive processes in nanofluids allowing access to, e.g., particle size and its distribution, dynamic light scattering (DLS) is the state-of-the-art technique. It is based on the analysis of microscopic fluctuations originating from the random thermal movement of particles in the continuous liquid phase at macroscopic thermodynamic equilibrium. For anisotropic particles or particle aggregates, besides translational diffusion also rotational diffusion occurs. To obtain the sum of the orientation-averaged translational (DT) and rotational (DR) diffusivities by depolarized DLS [2], a homodyne detection scheme is usually applied which can hardly be fulfilled in the experimental realization. Furthermore, the experiments are restricted to limited ranges for temperature, particle concentration, and viscosity

Thermodiffusion of the tetrahydronaphthalene and dodecane mixture under high pressure and in porous medium

A thermodiffusion cell is used in order to perform Soret experiments on binary mixtures at high pressure and in the presence of a porous medium. The cell is validated at atmospheric pressure with toluene/hexane and the tetrahydronaphthalene/dodecane mixtures. The mass separation follows a diffusive behaviour when the cell is filled with a porous medium. At least three times the relaxation time is needed to have a good estimation of the Soret coefficients. From the transient state of the mass separation and using accepted values of the diffusion coefficient, the tortuosity of the porous medium was evaluated, too. Finally, experiments at high pressure were performed with the tetrahydronaphthalene/dodecane system. In these experiments, decreases of the Soret coefficient and of the tortuosity of the porous medium were measured as a function of the pressure