F. Croccolo | Université De Pau Et Des Pays De L'adour (original) (raw)

Papers by F. Croccolo

npj Microgravity

The understanding of transport and mixing in fluids in the presence and in the absence of externa... more The understanding of transport and mixing in fluids in the presence and in the absence of external fields and reactions represents a challenging topic of strategic relevance for space exploration. Indeed, mixing and transport of components in a fluid are especially important during long-term space missions where fuels, food and other materials, needed for the sustainability of long space travels, must be processed under microgravity conditions. So far, the processes of transport and mixing have been investigated mainly at the macroscopic and microscopic scale. Their investigation at the mesoscopic scale is becoming increasingly important for the understanding of mass transfer in confined systems, such as porous media, biological systems and microfluidic systems. Microgravity conditions will provide the opportunity to analyze the effect of external fields and reactions on optimizing mixing and transport in the absence of the convective flows induced by buoyancy on Earth. This would b...

Microgravity Science and Technology, 2016

In a fluid system driven out of equilibrium by the presence of a gradient, fluctuations become lo... more In a fluid system driven out of equilibrium by the presence of a gradient, fluctuations become long-ranged and their intensity diverges at large spatial scales. This divergence is prevented vertical confinement and, in a stable configuration, by gravity. Gravity and confinement also affect the dynamics of non-equilibrium fluctuations (NEFs). In fact, small wavelength fluctuations decay diffusively, while the decay of long wavelength ones is either dominated by buoyancy or by confinement. In normal gravity, from the analysis of the dynamics one can extract the diffusion coefficients as well as other transport properties. For example, in a thermodiffusion experiment one can measure the Soret coefficient. Under microgravity, the relaxation of fluctuations occurs by diffusion only and this prevents the determination of the Soret coefficient of a binary mixture from the study of the dynamics. In this work we propose an innovative self-referencing optical method for the determination of the thermal diffusion 2 ratio of a binary mixture that does not require previous knowledge of the temperature difference applied to the sample. The method relies on the determination of the ratio between the mean squared amplitude of concentration and temperature fluctuations. We investigate data from the GRADFLEX experiment, an experiment flown onboard the Russian satellite FOTON M3 in 2007. The investigated sample is a suspension of polystyrene polymer chains (MW=9,100g/mol, concentration 1.8wt%) in toluene, stressed by different temperature gradients. The use of a quantitative shadowgraph technique allows to perform measurements in the absence of delicate alignment and calibration procedures. The statics of the concentration and temperature NEFs are obtained and their ratio is computed. At large wave vectors the ratio becomes constant and is shown to be proportional to the thermal diffusion ratio of the sample.

Microgravity Science and Technology, 2015

In this work we propose a methodology, based on molecular dynamics simulations, to quantify the i... more In this work we propose a methodology, based on molecular dynamics simulations, to quantify the influence of segregation and thermodiffusion on the initial state distribution of the fluid species in hydrocarbon reservoirs. This convection-free approach has been applied to a synthetic oil composed of three normal alkanes and to a real acid gas. It has been found that the thermodiffusion effect induced by the geothermal gradient is similar (but opposite in sign) to that due to segregation for both mixtures. In addition, because of the combined effect of thermal expansion and thermodiffusion, it has been observed that the density gradient can be reversed, in the presence of a geothermal gradient. These numerical results emphasize the need of improving our quantification of thermodiffusion in multicomponent mixtures. The SCCO-SJ10 experiments will be a crucial step towards this goal.

Polymer Degradation and Stability, 2008

A detailed study of argon plasma-induced graft-polymerisation of ethylene glycol methacrylate pho... more A detailed study of argon plasma-induced graft-polymerisation of ethylene glycol methacrylate phosphate (EGMP) on polyethylene (PE) substrates is presented. The process consists of four steps: (a) plasma pre-activation of the PE substrates; (b) immersion in an EGMP solution; (c) argon plasmainduced graft-polymerisation; (d) washing and drying of the samples. Influence of the solution and plasma parameters on the process efficiency, evaluated in terms of amount of grafted polymer and coverage uniformity, is investigated. The plasma-induced graft-polymerisation of EGMP is then followed by sample weighting, contact angle measurements, attenuated total reflection infrared (ATR-IR) spectroscopy and X-ray photoelectron spectroscopic (XPS) analysis. Finally, flame-retardant properties of modified PE substrates are evaluated by limiting oxygen index (LOI) measurements.

The Journal of Chemical Physics, 2011

In the present work binary mixtures of varying concentrations of two miscible hydrocarbons, 1,2,3... more In the present work binary mixtures of varying concentrations of two miscible hydrocarbons, 1,2,3,4tetrahydronaphtalene (THN) and n-dodecane (C12), are subjected to increasing pressure up to 50 MPa in order to investigate the dependence of the so-called concentration contrast factor (CF), i.e., (∂n/∂c) p,T , on pressure level. The refractive index is measured by means of a Mach-Zehnder interferometer. The setup and experimental procedure are validated with different pure fluids in the same pressure range. The refractive index of the THN-C12 mixture is found to vary both over pressure and concentration, and the concentration CF is found to exponentially decrease as the pressure is increased. The measured values of the refractive index and the concentration CFs are compared with values obtained by two different theoretical predictions, the well-known Lorentz-Lorenz formula and an alternative one proposed by Looyenga. While the measured refractive indices agree very well with predictions given by Looyenga, the measured concentration CFs show deviations from the latter of the order of 6% and more than the double from the Lorentz-Lorenz predictions.

Light scattering techniques are widely used in many fields of condensed and soft matter Physics. ... more Light scattering techniques are widely used in many fields of condensed and soft matter Physics. Usually these methods are based on the study of the scattered light in the far field. Recently, a new family of near field detection schemes has been developed, mainly for the study of small angle light scattering. These techniques are based on the detection of the light intensity close to the sample, where light scattered at different directions overlaps. Here we report data obtained with a near field scattering instrument, which performs measurements of both polarized and depolarized dynamic light scattering. Advantages of this procedure over the traditional far field detection include the immunity to stray light problems and the very large statistical sample simultaneously acquired for each measurement, at different wave vectors. By using the proposed technique we have measured the translational and rotational diffusion coefficients of rod-like colloidal particles, and the obtained data are in very good agreement with the data acquired with a traditional light scattering apparatus.

Anomalous Fluctuation Phenomena in Complex Systems: Plasmas, Fluids, and Financial Markets, C. Riccardi and HE Roman, eds.(Research Signpost, Trivandrum, 2008).[Citation Context], 2008

The European Physical Journal E, 2022

Microgravity Science and Technology, 2018

We report on thermodiffusion experiments conducted on the International Space Station ISS during ... more We report on thermodiffusion experiments conducted on the International Space Station ISS during fall 2016. These experiments are part of the DCMIX (Diffusion and thermodiffusion Coefficients Measurements in ternary Mixtures) project, which aims at establishing a reliable data base of non-isothermal transport coefficients for selected ternary liquid mixtures. The third campaign, DCMIX3, focuses on aqueous systems with water/ethanol/triethylene glycol as an example, where sign changes of the Soret coefficient have already been reported for certain binary subsystems. Investigations have been carried out with the SODI (Selectable Optical Diagnostics Instrument) instrument, a Mach-Zehnder interferometer set up inside the Microgravity Science Glovebox in the Destiny Module of the ISS. Concentration changes within the liquids have been monitored in response to an external temperature gradient using phase-stepping interferometry. The complete data set has been made available in spring 2017. Due to additionally available measurement time, it was possible to collect a complete data set at 30∘C and an almost complete data set at 25∘C, which significantly exceeds the originally envisaged measurements at a single temperature only. All samples could be measured successfully. The SODI instrument and the DCMIX experiments have proven reliable and robust, allowing to extract meaningful data even in case of unforeseen laser instabilities. First assessments of the data quality have revealed six out of 31 runs with some problems in image contrast and/or phase step stability that will require more sophisticated algorithms. This publication documents all relevant parameters of the conducted experiments and also events that might have an influence on the final results. The compiled information is intended to serve as a starting point for all following data evaluations.

The European Physical Journal E, 2016

Fluids in non-equilibrium steady states exhibit long-range fluctuations which extend over the ent... more Fluids in non-equilibrium steady states exhibit long-range fluctuations which extend over the entire system. They can be described by non-equilibrium thermodynamics and fluctuating hydrodynamics that assume local equilibrium for the thermophysical properties as a function of space and time. The experimental evidence for the consistency between this assumption of local equilibrium in the equations and the non-local fluctuation phenomena observed is reviewed.

The European physical journal. E, Soft matter, Dec 1, 2016

In a recent letter (C. Giraudet et al., EPL 111, 60013 (2015)) we reported preliminary data showi... more 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 analy...

Review of Scientific Instruments, 2011

New Journal of Physics, 2011

Comptes Rendus Mécanique, 2013

A thermodiffusion cell is used in order to perform Soret experiments on binary mixtures at high p... more 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.

Annals of the New York Academy of Sciences, 2006

Diffusion is commonly believed to be a homogeneous process at the mesoscopic scale, being driven ... more Diffusion is commonly believed to be a homogeneous process at the mesoscopic scale, being driven only by the random walk of fluid molecules. On the contrary, very large amplitude, long wavelength fluctuations always accompany diffusive processes. In the presence of gravity, fluctuations in a fluid containing a stabilizing gradient are affected by two different processes: diffusion, which relaxes them, and the buoyancy force, which quenches them. These phenomena affect both the overall amplitude of fluctuations and their time dependence. For the case of free diffusion, the time-correlation function of the concentration fluctuations is predicted to exhibit an exponential decay with correlation time depending on the wave vector q. For large wave vector fluctuations, diffusion dominates, and the correlation time is predicted to be 1 / (Dq2). For small wave vector fluctuations, gravitational forces have time to play a significant role, and the correlation time is predicted to be proportional to q2. The effects of gravity and diffusion are comparable for a critical wave vector q(c) determined by fluid properties and gravity. We have utilized a quantitative dynamic shadowgraph technique to obtain the temporal correlation function of a mixture of LUDOX(R) TMA and water undergoing free diffusion. This technique allows one to simultaneously measure correlation functions achieving good statistics for a number of different wave vectors in a single measurement. Wave vectors as small as 70 cm(-1) have been investigated, which is very difficult to achieve with ordinary dynamic light-scattering techniques. We present results on the transition from the diffusive decay of fluctuations to the regime in which gravity is dominant.

The European Physical Journal E, 2016

Diffusion and thermal diffusion processes in a liquid mixture are accompanied by long-range non-e... more Diffusion and thermal diffusion processes in a liquid mixture are accompanied by long-range non-equilibrium fluctuations, whose amplitude is orders of magnitude larger than that of equilibrium fluctuations. The mean square amplitude of the non-equilibrium fluctuations presents a scale-free power law behavior q −4 as a function of the wave vector q, but the divergence of the amplitude of the fluctuations at small wave vectors is prevented by the presence of gravity. In microgravity conditions the non-equilibrium fluctuations are fully developed and span all the available length scales up to the macroscopic size of the systems in the direction parallel to the applied gradient. Available theoretical models are based on linearized hydrodynamics and provide an adequate description of the statics and dynamics of the fluctuations in the presence of small temperature/concentration gradients and under stationary or quasi-stationary conditions. We describe a project aimed at the investigation of Non-EquilibriUm Fluctuations during DIffusion in compleX liquids (NEUF-DIX). The focus of the project is on the investigation of the non-equilibrium fluctuations in complex liquids, trying to tackle several challenging problems that emerged during the latest years, such as the theoretical predictions of Casimir-like forces induced by non-equilibrium fluctuations; the understanding of the non-equilibrium fluctuations in multi-component mixtures including a polymer, both in relation to the transport coefficients and to their behavior close to a glass transition; the understanding of the non-equilibrium fluctuations in concentrated colloidal suspensions, a problem closely related with the detection of Casimir forces; and the investigation of the onset of fluctuations during transient diffusion. We envision to parallel these experiments with state of the art multi-scale simulations.

The European Physical Journal E

We investigate by dynamic shadowgraphy the non-equilibrium fluctuations at the steady state of a ... more We investigate by dynamic shadowgraphy the non-equilibrium fluctuations at the steady state of a thermodiffusion experiment in a polymeric ternary mixture of polystyrene-toluene-nhexane. The structure function of the refractive index reveals the existence of quite different decay times, thus requiring the analysis of a wide range of correlation times. This is related to the simultaneous presence of three distinct decay modes corresponding to (from fastest to slowest) relaxation of temperature fluctuations, of the concentration fluctuations of the mixed solvent, and of the concentration fluctuations of the polymer in the binary solvent. An investigation of the decay times at the corresponding diffusive regimes provides a measurement of the thermal diffusivity and the two eigenvalues of the mass diffusion matrix of the ternary mixture. Similar experiments were performed in the past but here, to suppress the confinement effect and obtain a more direct comparison with the theory, a thicker sample is studied. Moreover, also a faster camera is used allowing the experimental observation of faster modes, like the propagative ones. The experimental values of the decay times are eventually compared with those predicted by different available theories. Finally, we present a more complete theoretical model to describe the non-equilibrium fluctuations in the bulk of a ternary mixture at the steady state of a thermodiffusion experiment.

The European Physical Journal E

This paper describes the European Space Agency (ESA) experiments devoted to study thermodiffusion... more 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.

npj Microgravity

The understanding of transport and mixing in fluids in the presence and in the absence of externa... more The understanding of transport and mixing in fluids in the presence and in the absence of external fields and reactions represents a challenging topic of strategic relevance for space exploration. Indeed, mixing and transport of components in a fluid are especially important during long-term space missions where fuels, food and other materials, needed for the sustainability of long space travels, must be processed under microgravity conditions. So far, the processes of transport and mixing have been investigated mainly at the macroscopic and microscopic scale. Their investigation at the mesoscopic scale is becoming increasingly important for the understanding of mass transfer in confined systems, such as porous media, biological systems and microfluidic systems. Microgravity conditions will provide the opportunity to analyze the effect of external fields and reactions on optimizing mixing and transport in the absence of the convective flows induced by buoyancy on Earth. This would b...

Microgravity Science and Technology, 2016

In a fluid system driven out of equilibrium by the presence of a gradient, fluctuations become lo... more In a fluid system driven out of equilibrium by the presence of a gradient, fluctuations become long-ranged and their intensity diverges at large spatial scales. This divergence is prevented vertical confinement and, in a stable configuration, by gravity. Gravity and confinement also affect the dynamics of non-equilibrium fluctuations (NEFs). In fact, small wavelength fluctuations decay diffusively, while the decay of long wavelength ones is either dominated by buoyancy or by confinement. In normal gravity, from the analysis of the dynamics one can extract the diffusion coefficients as well as other transport properties. For example, in a thermodiffusion experiment one can measure the Soret coefficient. Under microgravity, the relaxation of fluctuations occurs by diffusion only and this prevents the determination of the Soret coefficient of a binary mixture from the study of the dynamics. In this work we propose an innovative self-referencing optical method for the determination of the thermal diffusion 2 ratio of a binary mixture that does not require previous knowledge of the temperature difference applied to the sample. The method relies on the determination of the ratio between the mean squared amplitude of concentration and temperature fluctuations. We investigate data from the GRADFLEX experiment, an experiment flown onboard the Russian satellite FOTON M3 in 2007. The investigated sample is a suspension of polystyrene polymer chains (MW=9,100g/mol, concentration 1.8wt%) in toluene, stressed by different temperature gradients. The use of a quantitative shadowgraph technique allows to perform measurements in the absence of delicate alignment and calibration procedures. The statics of the concentration and temperature NEFs are obtained and their ratio is computed. At large wave vectors the ratio becomes constant and is shown to be proportional to the thermal diffusion ratio of the sample.

Microgravity Science and Technology, 2015

In this work we propose a methodology, based on molecular dynamics simulations, to quantify the i... more In this work we propose a methodology, based on molecular dynamics simulations, to quantify the influence of segregation and thermodiffusion on the initial state distribution of the fluid species in hydrocarbon reservoirs. This convection-free approach has been applied to a synthetic oil composed of three normal alkanes and to a real acid gas. It has been found that the thermodiffusion effect induced by the geothermal gradient is similar (but opposite in sign) to that due to segregation for both mixtures. In addition, because of the combined effect of thermal expansion and thermodiffusion, it has been observed that the density gradient can be reversed, in the presence of a geothermal gradient. These numerical results emphasize the need of improving our quantification of thermodiffusion in multicomponent mixtures. The SCCO-SJ10 experiments will be a crucial step towards this goal.

Polymer Degradation and Stability, 2008

A detailed study of argon plasma-induced graft-polymerisation of ethylene glycol methacrylate pho... more A detailed study of argon plasma-induced graft-polymerisation of ethylene glycol methacrylate phosphate (EGMP) on polyethylene (PE) substrates is presented. The process consists of four steps: (a) plasma pre-activation of the PE substrates; (b) immersion in an EGMP solution; (c) argon plasmainduced graft-polymerisation; (d) washing and drying of the samples. Influence of the solution and plasma parameters on the process efficiency, evaluated in terms of amount of grafted polymer and coverage uniformity, is investigated. The plasma-induced graft-polymerisation of EGMP is then followed by sample weighting, contact angle measurements, attenuated total reflection infrared (ATR-IR) spectroscopy and X-ray photoelectron spectroscopic (XPS) analysis. Finally, flame-retardant properties of modified PE substrates are evaluated by limiting oxygen index (LOI) measurements.

The Journal of Chemical Physics, 2011

In the present work binary mixtures of varying concentrations of two miscible hydrocarbons, 1,2,3... more In the present work binary mixtures of varying concentrations of two miscible hydrocarbons, 1,2,3,4tetrahydronaphtalene (THN) and n-dodecane (C12), are subjected to increasing pressure up to 50 MPa in order to investigate the dependence of the so-called concentration contrast factor (CF), i.e., (∂n/∂c) p,T , on pressure level. The refractive index is measured by means of a Mach-Zehnder interferometer. The setup and experimental procedure are validated with different pure fluids in the same pressure range. The refractive index of the THN-C12 mixture is found to vary both over pressure and concentration, and the concentration CF is found to exponentially decrease as the pressure is increased. The measured values of the refractive index and the concentration CFs are compared with values obtained by two different theoretical predictions, the well-known Lorentz-Lorenz formula and an alternative one proposed by Looyenga. While the measured refractive indices agree very well with predictions given by Looyenga, the measured concentration CFs show deviations from the latter of the order of 6% and more than the double from the Lorentz-Lorenz predictions.

Light scattering techniques are widely used in many fields of condensed and soft matter Physics. ... more Light scattering techniques are widely used in many fields of condensed and soft matter Physics. Usually these methods are based on the study of the scattered light in the far field. Recently, a new family of near field detection schemes has been developed, mainly for the study of small angle light scattering. These techniques are based on the detection of the light intensity close to the sample, where light scattered at different directions overlaps. Here we report data obtained with a near field scattering instrument, which performs measurements of both polarized and depolarized dynamic light scattering. Advantages of this procedure over the traditional far field detection include the immunity to stray light problems and the very large statistical sample simultaneously acquired for each measurement, at different wave vectors. By using the proposed technique we have measured the translational and rotational diffusion coefficients of rod-like colloidal particles, and the obtained data are in very good agreement with the data acquired with a traditional light scattering apparatus.

Anomalous Fluctuation Phenomena in Complex Systems: Plasmas, Fluids, and Financial Markets, C. Riccardi and HE Roman, eds.(Research Signpost, Trivandrum, 2008).[Citation Context], 2008

The European Physical Journal E, 2022

Microgravity Science and Technology, 2018

We report on thermodiffusion experiments conducted on the International Space Station ISS during ... more We report on thermodiffusion experiments conducted on the International Space Station ISS during fall 2016. These experiments are part of the DCMIX (Diffusion and thermodiffusion Coefficients Measurements in ternary Mixtures) project, which aims at establishing a reliable data base of non-isothermal transport coefficients for selected ternary liquid mixtures. The third campaign, DCMIX3, focuses on aqueous systems with water/ethanol/triethylene glycol as an example, where sign changes of the Soret coefficient have already been reported for certain binary subsystems. Investigations have been carried out with the SODI (Selectable Optical Diagnostics Instrument) instrument, a Mach-Zehnder interferometer set up inside the Microgravity Science Glovebox in the Destiny Module of the ISS. Concentration changes within the liquids have been monitored in response to an external temperature gradient using phase-stepping interferometry. The complete data set has been made available in spring 2017. Due to additionally available measurement time, it was possible to collect a complete data set at 30∘C and an almost complete data set at 25∘C, which significantly exceeds the originally envisaged measurements at a single temperature only. All samples could be measured successfully. The SODI instrument and the DCMIX experiments have proven reliable and robust, allowing to extract meaningful data even in case of unforeseen laser instabilities. First assessments of the data quality have revealed six out of 31 runs with some problems in image contrast and/or phase step stability that will require more sophisticated algorithms. This publication documents all relevant parameters of the conducted experiments and also events that might have an influence on the final results. The compiled information is intended to serve as a starting point for all following data evaluations.

The European Physical Journal E, 2016

Fluids in non-equilibrium steady states exhibit long-range fluctuations which extend over the ent... more Fluids in non-equilibrium steady states exhibit long-range fluctuations which extend over the entire system. They can be described by non-equilibrium thermodynamics and fluctuating hydrodynamics that assume local equilibrium for the thermophysical properties as a function of space and time. The experimental evidence for the consistency between this assumption of local equilibrium in the equations and the non-local fluctuation phenomena observed is reviewed.

The European physical journal. E, Soft matter, Dec 1, 2016

In a recent letter (C. Giraudet et al., EPL 111, 60013 (2015)) we reported preliminary data showi... more 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 analy...

Review of Scientific Instruments, 2011

New Journal of Physics, 2011

Comptes Rendus Mécanique, 2013

A thermodiffusion cell is used in order to perform Soret experiments on binary mixtures at high p... more 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.

Annals of the New York Academy of Sciences, 2006

Diffusion is commonly believed to be a homogeneous process at the mesoscopic scale, being driven ... more Diffusion is commonly believed to be a homogeneous process at the mesoscopic scale, being driven only by the random walk of fluid molecules. On the contrary, very large amplitude, long wavelength fluctuations always accompany diffusive processes. In the presence of gravity, fluctuations in a fluid containing a stabilizing gradient are affected by two different processes: diffusion, which relaxes them, and the buoyancy force, which quenches them. These phenomena affect both the overall amplitude of fluctuations and their time dependence. For the case of free diffusion, the time-correlation function of the concentration fluctuations is predicted to exhibit an exponential decay with correlation time depending on the wave vector q. For large wave vector fluctuations, diffusion dominates, and the correlation time is predicted to be 1 / (Dq2). For small wave vector fluctuations, gravitational forces have time to play a significant role, and the correlation time is predicted to be proportional to q2. The effects of gravity and diffusion are comparable for a critical wave vector q(c) determined by fluid properties and gravity. We have utilized a quantitative dynamic shadowgraph technique to obtain the temporal correlation function of a mixture of LUDOX(R) TMA and water undergoing free diffusion. This technique allows one to simultaneously measure correlation functions achieving good statistics for a number of different wave vectors in a single measurement. Wave vectors as small as 70 cm(-1) have been investigated, which is very difficult to achieve with ordinary dynamic light-scattering techniques. We present results on the transition from the diffusive decay of fluctuations to the regime in which gravity is dominant.

The European Physical Journal E, 2016

Diffusion and thermal diffusion processes in a liquid mixture are accompanied by long-range non-e... more Diffusion and thermal diffusion processes in a liquid mixture are accompanied by long-range non-equilibrium fluctuations, whose amplitude is orders of magnitude larger than that of equilibrium fluctuations. The mean square amplitude of the non-equilibrium fluctuations presents a scale-free power law behavior q −4 as a function of the wave vector q, but the divergence of the amplitude of the fluctuations at small wave vectors is prevented by the presence of gravity. In microgravity conditions the non-equilibrium fluctuations are fully developed and span all the available length scales up to the macroscopic size of the systems in the direction parallel to the applied gradient. Available theoretical models are based on linearized hydrodynamics and provide an adequate description of the statics and dynamics of the fluctuations in the presence of small temperature/concentration gradients and under stationary or quasi-stationary conditions. We describe a project aimed at the investigation of Non-EquilibriUm Fluctuations during DIffusion in compleX liquids (NEUF-DIX). The focus of the project is on the investigation of the non-equilibrium fluctuations in complex liquids, trying to tackle several challenging problems that emerged during the latest years, such as the theoretical predictions of Casimir-like forces induced by non-equilibrium fluctuations; the understanding of the non-equilibrium fluctuations in multi-component mixtures including a polymer, both in relation to the transport coefficients and to their behavior close to a glass transition; the understanding of the non-equilibrium fluctuations in concentrated colloidal suspensions, a problem closely related with the detection of Casimir forces; and the investigation of the onset of fluctuations during transient diffusion. We envision to parallel these experiments with state of the art multi-scale simulations.

The European Physical Journal E

We investigate by dynamic shadowgraphy the non-equilibrium fluctuations at the steady state of a ... more We investigate by dynamic shadowgraphy the non-equilibrium fluctuations at the steady state of a thermodiffusion experiment in a polymeric ternary mixture of polystyrene-toluene-nhexane. The structure function of the refractive index reveals the existence of quite different decay times, thus requiring the analysis of a wide range of correlation times. This is related to the simultaneous presence of three distinct decay modes corresponding to (from fastest to slowest) relaxation of temperature fluctuations, of the concentration fluctuations of the mixed solvent, and of the concentration fluctuations of the polymer in the binary solvent. An investigation of the decay times at the corresponding diffusive regimes provides a measurement of the thermal diffusivity and the two eigenvalues of the mass diffusion matrix of the ternary mixture. Similar experiments were performed in the past but here, to suppress the confinement effect and obtain a more direct comparison with the theory, a thicker sample is studied. Moreover, also a faster camera is used allowing the experimental observation of faster modes, like the propagative ones. The experimental values of the decay times are eventually compared with those predicted by different available theories. Finally, we present a more complete theoretical model to describe the non-equilibrium fluctuations in the bulk of a ternary mixture at the steady state of a thermodiffusion experiment.

The European Physical Journal E

This paper describes the European Space Agency (ESA) experiments devoted to study thermodiffusion... more 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.