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Interactions effectives et dynamiques en systèmes actifs de colloïdes autopropulsés

Abstract : This project aimed to systematically investigate the interactions, microstructure and dynamics in suspensions of colloidal particles that mimic active motions, using (Ultra) Small- Angle X-ray Scattering (USAXS/SAXS) and X-ray Photon Correlation Spectroscopy (XPCS). As opposed to the conventional passive colloids (Brownian particles), active colloids are non-equilibrium systems consisting of self-propelled particles that display many fascinating dynamics, such as streaming, swarming, flocking, etc. in appropriate media. Practical examples of active systems are motile microorganisms, such as some species of bacteria, or synthetic Janus colloids – characterized by an asymmetric chemical composition of their surface – that can induce a propulsion mechanisms, like self-diffusiophoresis. The foci of this thesis are on interparticle interactions, particle-medium interactions and the phoretic dynamics in active systems.Firstly, the structure and motility of Escherichia coli bacteria were investigated by combined USAXS and SAXS methods. As an offshoot, the scattering data spanning a broad scattering vector (q)-range permitted the derivation of a multiscale structural model by combining colloidal (cell-body), membrane (cell-envelope) and polymer (flagella) features. This model was further refined by contrast-variation Small Angle Neutron Scattering (SANS) measurements on E. coli suspensions at three match points and the full contrast which allowed the determination of the membrane electron-density and the inter-membrane distances on a quantitative scale.These bacteria were then used as active component in a mixture with micron-sized passive silica colloids, with the aim of investigating how the effective interactions and dynamics of passive colloids are affected by the presence and the motility of active E. coli. Both static and hydrodynamic information were obtained via the simultaneous use of USAXS and XPCS techniques. Data suggested active bacteria act as a fluidizing agent in such systems, reducing attractive interactions and enhancing the dynamics of passive colloids, which, at the same time, are affected by the buffer and more viscous environment due to the bacterial presence.Finally, the phoretic motions of micron-sized silica colloids and half-coated silica/nickel Janus colloids suspended in a mixture of 3-methylpyridine (3MP) and water/heavy water undergoing liquid-liquid phase separation were investigated using USAXS and XPCS. Due to the preferential wetting of 3MP on the silica surface, the motion of the colloids is strongly correlated to the dynamics of phase separation.Silica colloids displayed advective motion with enhanced diffusion toward the 3MP-rich phase reminiscent of self-propelled motion until the phase separation is completed. Suspensions of Janus colloids showed a much richer scenario, where colloid dynamics are strongly influenced by the asymmetric interactions with the solvent. The dynamics of Janus colloids were either enhanced or suppressed depending on the 3MP concentration, which, concurrently, affected the microstructure of the system. As opposed to the partitioning in 3MP-rich phase in the case of silica colloids, Janus particles behave like surfactants at the interface.The thesis demonstrates the ability of studying active systems by means of scattering methods and probe their behaviour in the thermodynamic limit and complement the information derived from direct microscopy observations.
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Enrico Federico Semeraro. Interactions effectives et dynamiques en systèmes actifs de colloïdes autopropulsés. Biochimie, Biologie Moléculaire. Université Grenoble Alpes, 2017. Français. ⟨NNT : 2017GREAV017⟩. ⟨tel-01686239⟩

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