European Space Agency experiments on thermodiffusion of fluid mixtures in space.

This paper describes the European Space Agency (ESA) experiments devoted to study thermodiffusion of fluid mixtures in microgravity environment, where sedimentation and convection do not affect the mass flow induced by the Soret effect. First, the experiments performed on binary mixtures in the IVIDIL and GRADFLEX experiments are described. Then, further experiments on ternary mixtures and complex fluids performed in DCMIX and planned to be performed in the context of the NEUF-DIX project are presented. Finally, multi-component mixtures studied in the SCCO project are detailed.

Development of a high-pressure set-up for measurements of binary diffusion coefficients in supercritical carbon dioxide.

We present the development of a high-pressure apparatus for measurements of diffusion coefficients in supercritical fluids. The Taylor dispersion method has been adapted to conduct experiments at the pressures up to 25.0 MPa. In order to test the developed set-up, binary diffusion coefficients D at infinite dilution in supercritical carbon dioxide have been measured for a reference system, benzene, at temperatures in the range of 309.50-319.95 K. The effects of flow velocity, number of consecutive injections and absorbance at different wave numbers on the diffusion coefficient have been analysed. The obtained diffusion coefficients are of the order of 10-8 m 2/s and in excellent agreement with the available literature data.

Fickian Diffusion in Ternary Mixtures Composed by 1,2,3,4-Tetrahydronaphthalene, Isobutylbenzene, and n-Dodecane.

We report the Fickian diffusion coefficients in 20 ternary mixtures formed by 1,2,3,4-tetrahydronaphthalene (THN), isobutylbenzene (IBB) and n-dodecane (nC12) measured by the Taylor dispersion technique at 298.1 K and atmospheric pressure. Four diffusion coefficients of the ternary mixtures were measured along six concentration paths starting on one binary subsystem and moving toward the other one. We found expressions for the diffusion matrix of a ternary mixture approaching to the binary limits. The measured diffusion coefficients were thoroughly verified by comparison with the theoretical asymptotic behavior. The main diffusion coefficients vary smoothly over the entire concentration space and D11 is always larger than D22. One of the two cross-diffusion coefficients is of the same order of magnitude as the main ones and, hence, not negligible, whereas the other one is close to zero. The investigated mixtures also comprise compositions that were examined in microgravity experiments in the ESA DCMIX1 project.

Investigation of Fickian diffusion in the ternary mixtures of water-ethanol-triethylene glycol and its binary pairs.

We present a comprehensive experimental study of isothermal Fickian diffusion in the ternary and binary liquid mixtures of water, ethanol, and triethylene glycol over the entire ternary composition space. 21 ternary mixtures inside the composition triangle have been investigated by means of the Taylor dispersion technique and 30 binary mixtures by Taylor dispersion and/or optical beam deflection in a Soret cell. The scalar binary diffusion coefficient has been determined along all three binary boundaries of the composition space and compared with estimations based on the Stokes-Einstein relation using stick or slip boundary conditions. The four elements of the ternary diffusion matrix and the diffusion eigenvalues were determined over a large portion of the composition triangle. The pseudo-binary diffusion coefficients obtained in Taylor dispersion experiments with either one of the two independent concentrations kept constant are comparable to the two diffusion eigenvalues. One of the two off-diagonal elements of the diffusion matrix is of the same order as the diagonal ones and, hence, not negligible, whereas the other one is approximately one order of magnitude smaller. Where available, our results compare well with literature data. The investigated compositions also comprise the five compositions that are scheduled for microgravity experiments in the ESA DCMIX3 project.

Contribution to the benchmark for ternary mixtures: Measurement of the Soret, diffusion and thermodiffusion coefficients in the ternary mixture THN/IBB/nC12 with 0.8/0.1/0.1 mass fractions in ground and orbital laboratories.

We have determined the Soret (ST), diffusion (D, and thermodiffusion (DT) coefficients in a ternary mixture of tetralin-isobutylbenzene-n-dodecane with a composition of 0.80/0.10/0.10 by mass fraction at a temperature of 298K. The Soret coefficients were measured in the microgravity experiment DCMIX1 and on the ground by optical digital interferometry (ODI) using two lasers with different wavelengths. The values of the Soret coefficients were determined from the stationary separation of the components using two- and six-parameter fits. The diffusion coefficients were independently measured using the Taylor Dispersion Technique in the ground laboratory, and the thermodiffusion coefficients were derived from known ST and matrix D. The processing of the data from the DCMIX experiment conducted on the International Space Station is discussed in detail. The multi-user design of the on-board instrument causes perturbations in the component separation. Several recommendations are suggested for improving the quality of the microgravity results. For example, we demonstrated that the tomography reconstruction of the 3-D concentration field allows to restore the underestimated component separation resulting from the spatial non-linearity of the temperature field. Furthermore, to avoid errors in component separation due to mass exchange between the working liquid volume and the expansion volume at the top of the cell, we suggest considering the evolution of the separation only in the lower half of the cell. The results of this study displayed reasonable quantitative agreement between the microgravity and ground experiments.

Benchmark values for the Soret, thermodiffusion and molecular diffusion coefficients of the ternary mixture tetralin+isobutylbenzene+n-dodecane with 0.8-0.1-0.1 mass fraction.

With the aim of providing reliable benchmark values, we have measured the Soret, thermodiffusion and molecular diffusion coefficients for the ternary mixture formed by 1,2,3,4-tetrahydronaphthalene, isobutylbenzene and n-dodecane for a mass fraction of 0.8-0.1-0.1 and at a temperature of 25°C. The experimental techniques used by the six participating laboratories are Optical Digital Interferometry, Taylor Dispersion technique, Open Ended Capillary, Optical Beam Deflection, Thermogravitational technique and Sliding Symmetric Tubes technique in ground conditions and Selectable Optical Diagnostic Instrument (SODI) in microgravity conditions. The measurements obtained in the SODI installation have been analyzed independently by four laboratories. Benchmark values are proposed for the thermodiffusion and Soret coefficients and for the eigenvalues of the diffusion matrix in ground conditions, and for Soret coefficients in microgravity conditions.

Soret separation in a binary liquid mixture near its critical temperature.

The values of transport coefficients near a critical point are typically enhanced compared to the values in the classical region far away from a critical point. We report on the impact of the asymptotic behavior of the mass diffusion near the critical region on the Soret separation of the components in a model binary mixture. Concentration patterns are numerically investigated in the case of a spatially varying temperature. The Soret separation in ordinary mixture leads to the establishing of a linear concentration distribution in a steady state. The presence of the critical point redistributes the concentration field, it creates a thin layer with sharp concentration change at the critical region which can be seen as a horizontal plateau on vertical profiles. Large concentration gradients are established across this layer. The analysis showed that the kinetic of the separation significantly depends on whether the critical temperature is inside or outside of the applied temperature region, which is T(cold) ≤ T ≤ T(hot). Critical separation road is suggested for the case when T(cr) is located inside this region, T(cold) ≤ T(cr) ≤ T(hot).

Investigation of Fickian diffusion in the ternary mixture of 1,2,3,4-tetrahydronaphthalene, isobutylbenzene, and dodecane.

We present a comprehensive analysis of experimental results obtained for Fickian diffusion in the benchmark ternary liquid mixture of 1,2,3,4-tetrahydronaphthalene, isobutylbenzene, and dodecane (nC12) with equal mass fractions. Isothermal diffusion coefficients have been measured by two independent experimental methods: by Taylor dispersion technique, and by a counter flow cell fitted with an optical interferometry device. The experimental diffusion matrices have been critically analyzed regarding the Onsager reciprocal relations, for which we introduce a matrix asymmetry index s(2) that is independent of the frame of reference and the component order.

Impact of conditions at start-up on thermovibrational convective flow.

The development of thermovibrational convection in a cubic cell filled with high Prandtl number liquid (isopropanol) is studied. Direct nonlinear simulations are performed by solving three-dimensional Navier-Stokes equations in the Boussinesq approximation. The cell is subjected to high frequency periodic oscillations perpendicular to the applied temperature gradient under zero gravity. Two types of vibrations are imposed: either as a sine or cosine function of time. It is shown that the initial vibrational phase plays a significant role in the transient behavior of thermovibrational convective flow. Such knowledge is important to interpret correctly short-duration experimental results performed in microgravity, among which the most accessible are drop towers ( approximately 5s) and parabolic flights ( approximately 20s) . It is obtained that under sine vibrations, the flow reaches steady state within less than one thermal time. Under cosine acceleration, this time is 2 times longer. For cosine excitations, the Nusselt number is approximately 10 times smaller in comparison with the sine case. Besides, in the case of cosine, the Nusselt number oscillates with double frequency. However, at the steady state, time-averaged and oscillatory characteristics of the flow are independent of the vibrational start-up. The only feature that always differs the two cases is the phase difference between the velocity, temperature, and accelerations. We have found that due to nonlinear response of the system to the imposed vibrations, the phase shift between velocity and temperature is never equal exactly to pi2 , at least in weightlessness. Thus, heat transport always exists from the beginning of vibrations, although it might be weak.

Nonlinear Marangoni convection with the inclined temperature gradient in multilayer systems.

The influence of the horizontal component of the temperature gradient on nonlinear regimes of oscillatory Marangoni convection in a real symmetric three-layer system is investigated. The transitions between different flow regimes have been studied. The general diagram of regimes is constructed.

Onset of convection in Soret-driven instability.

It is common knowledge that light fluids rise while heavy fluids sink in the gravity field. The most obvious case is the isothermal Rayleigh-Taylor instability when a heavy fluid is placed on top of a light one. In the nonisothermal case, while heating from above, the density stratification is stable in a pure liquid. However, unstable density stratification might be established in a binary mixture with a negative Soret effect in the case of heating from above: the heavier liquid is accumulated on the top of the lighter one. Due to the large differences between viscous, thermal, and diffusion times the system has a tendency to fingering buoyant instabilities. At some moment the flow may be initiated. Near the onset of convection the flow pattern has a columnar convective structure: for a relatively low applied temperature difference Delta T the lighter and colder liquid is drawn up in the central part of the cell and the heavier liquid flows down along the walls. For finite size systems the situation is reversed at higher Delta T. Here we present results of three-dimensional direct numerical simulations of heat and mass transfer in a system with a negative Soret effect. While the development of Soret-induced convection is similar for a wide class of liquids: water based mixtures, colloidal, and polymer solutions, the parameters of the chosen system correspond to a realistic binary mixture of water (90%) and isopropanol (10%) enabling comparison of theoretical predictions with planned experimental studies.

Improvement in visibility of an in-focus reconstructed image in digital holography by reduction of the influence of out-of-focus objects.

When a reconstruction is performed on a digital holographic image that contains small objects at different depths, diffraction that is due to out-of-focus objects disrupts the visibility of the nearby focused objects. We propose a method to substitute for focused object amplitudes other amplitudes that will reduce propagation diffraction effects when other depths are investigated. The replacement amplitudes are computed by use of an algorithm that reduces the highest spatial frequencies of the resultant image. The theoretical aspects of the method are presented, and results for simulated and experimental examples are shown.

Interfacial nonequilibrium and Bénard-Marangoni instability of a liquid-vapor system.

We study Bénard-Marangoni instability in a system formed by a horizontal liquid layer and its overlying vapor. The liquid is lying on a hot rigid plate and the vapor is bounded by a cold parallel plate. A pump maintains a reduced pressure in the vapor layer and evacuates the vapor. This investigation is undertaken within the classical quasisteady approximation for both the vapor and the liquid phases. The two layers are separated by a deformable interface. Temporarily frozen temperature and velocity distributions are employed at each instant for the stability analysis, limited to infinitesimal disturbances (linear regime). We use irreversible thermodynamics to model the phase change under interfacial nonequilibrium. Within this description, the interface appears as a barrier for transport of both heat and mass. Hence, in contrast with previous studies, we consider the possibility of a temperature jump across the interface, as recently measured experimentally. The stability analysis shows that the interfacial resistances to heat and mass transfer have a destabilizing influence compared to an interface that is in thermodynamic equilibrium. The role of the fluctuations in the vapor phase on the onset of instability is discussed. The conditions to reduce the system to a one phase model are also established. Finally, the influence of the evaporation parameters and of the presence of an inert gas on the marginal stability curves is discussed.

Multistability of oscillatory thermocapillary convection in a liquid bridge.

A parametric investigation of the onset of chaos in a liquid bridge was numerically carried out for a medium Prandtl number liquid, Pr = 4, and unit aspect ratio under zero-gravity conditions. Spatiotemporal patterns of thermocapillary flow were successively studied beginning from the onset of instability up to the appearance of the nonperiodic flow and further on. Well-tested numerical code is used for solving the three-dimensional time-dependent Navier-Stokes equations in cylindrical coordinate system. Two-dimensional steady flow becomes oscillatory with azimuthal wave number m=2 as a result of Hopf bifurcation at Re(cr)(1)=630. A second independent solution with wave number m=3 was found to appear at Reynolds number Re(cr)(2) approximately 810. Two branches of three-dimensional periodic orbits, traveling waves with m=2 and m=3, coexist for Re>Re(cr)(2). Additional stable branches do not connect them. The different flow organizations reveal different behaviors in the supercritical area. The m=2 traveling wave always remains periodic, but the mode m=3 starts exhibiting chaotic features at Re approximately 4200. The onset of temporal nonperiodicity was shown to be associated with development of broadband noise in spectra and preceded by a quasiperiodicity. The flow stabilizes back to periodic with single frequency when Re exceeds a value Re approximately 5100. The window of periodicity exists up to at least Re=6000, the largest investigated value of the Reynolds number.

Thermocapillary-buoyancy convection in a shallow cavity heated from the side.

Combined thermocapillary-buoyancy convection has been investigated numerically in an extended cavity with differently heated walls. When the Marangoni number Ma grows, the unicellular flow is replaced by a steady bicellular or multicellular flow and then either by a hydrothermal wave or an oscillatory multicellular flow, depending on the dynamic Bond number Bo(dyn). The appearance of a hydrothermal wave prevents the propagation of the stationary roll structure, which spreads from the hot side, over the whole cavity. The hydrothermal wave itself looks as a succession of the cells moving from the cold side towards the motionless rolls on the hot side. For an intermediate interval of Bo(dyn) the parallel flow is unstable with respect to the hydrothermal wave (HTW), but the multicellular periodic structure generated by the side-wall perturbation is stable, so that the HTW decays in space when propagating on the background of the multicellular structure. The nonlinear competition between finite-amplitude, boundary-induced steady patterns and hydrothermal waves is essential. A nonlinear simulation of flow regimes in a wide region of the values of dynamical Bond number and Marangoni number is presented. A number of phenomena that cannot be predicted in the framework of the linear stability theory, specifically those characteristic for the motion in the intermediate interval of Bo(dyn), as well as the secondary transition from steady to unsteady flows at large Bo(dyn), which takes place when the Marangoni number Ma grows, are described.

Pattern recognition with a digital holographic microscope working in partially coherent illumination.

We describe the implementation of the automatic spatial-frequency-selection filter for recognition of patterns obtained with a digital holographic microscope working with a partially coherent source. The microscope provides the complex-optical-amplitude field that allows a refocusing plane-by-plane of the sample under investigation by numerical computation of the optical propagation. By inserting a correlation filter in the propagation equation, the correlation between the filter and the propagated optical field is obtained. In this way, the pattern is located in the direction of the optical axis. Owing to the very weak noise level generated by the partially coherent source, the correlation process is shift invariant. Therefore the samples can be located in the three dimensions. To have a robust recognition process, a generalized version of the automatic spatial-frequency-selection filters has been implemented. The method is experimentally demonstrated in a two-class problem for the recognition of protein crystals.

Border processing in digital holography by extension of the digital hologram and reduction of the higher spatial frequencies.

When a digital holographic reconstruction is performed, digital diffraction effects occur at the borders when the hologram amplitudes at the two opposite border points are different on each vertical or horizontal line. We propose a method of digital hologram extension to reduce such diffraction effects. The method consists of extending the size of the digital hologram and of filling the extended part by complex values that minimize, according to a numerical criterion, the highest spatial frequencies. The theoretical aspects of the method are given and the results from a demonstration are provided.

Anticonvection with an inclined temperature gradient.

Anticonvection, caused by external heating from above in the presence of heat sources (or sinks) homogeneously distributed on the interface, is investigated in the presence of an imposed horizontal temperature gradient. Numerical finite-difference simulations of the finite-amplitude convective regimes have been performed for the two-layer system of fluids. The interface is assumed to be flat. We discuss different scenarios of transition between multicell regimes characteristic of a vertical temperature gradient, and unicell structures induced by horizontal gradients. The coexistence of these two regimes in sufficiently long cavities has been obtained. Regular oscillations are also predicted in other situations.

Improved three-dimensional imaging with a digital holography microscope with a source of partial spatial coherence.

A digital holographic technique is implemented in a microscope for three-dimensional imaging reconstruction. The setup is a Mach-Zehnder interferometer that uses an incoherent light source to remove the coherent noise that is inherent in the laser sources. A phase-stepping technique determines the optical phase in the image plane of the microscope. Out-of-focus planes are refocused by digital holographic computations, thus considerably enlarging the depth of investigation without the need to change the optical focus mechanically. The technique can be implemented in transmission for various magnification ratios and can cover a wide range of applications. Performances and limitations of the microscope are theoretically evaluated. Experimental results for a test target are given, and examples of two applications in particle localization and investigation of biological sample are provided.