We present both the experimental and computational methods and results of phase-separating experiments performed with sulfur hexafluoride (SF6) close to its critical density. These experiments were performed in microgravity to suppress buoyancy and convection-driven effects. Phase separation under reduced gravity is analyzed for both 0.3 mK and 3.6 mK temperature quenches in order to derive the early-stage growth law. We found a 1/3 growth law for early stages of phase separation for a volume fraction of minority domains of 50%. Our findings support the hypothesis of a crossover between Brownian motion and hydrodynamic effects in the early stages of phase separation. The temperature inside the bulk of the pure fluid was estimated using a proposed histogram method. Our histogram method allowed temperature estimation below thermistors' sensitivity and detected small temperature variations inside the bulk of the pure fluid.
Large density fluctuations were observed by illuminating a cylindrical cell filled with sulfur hexafluoride (SF(6)), very near its liquid-gas critical point (|T-T(c)|< 300 μK) and recorded using a microscope with 3 μm spatial resolution. Using a dynamic structure factor algorithm, we determined from the recorded images the structure factor (SF), which measures the spatial distribution of fluctuations at different moments, and the correlation time of fluctuations. This method authorizes local measurements in contrast to the classical scattering techniques that average fluctuations over the illuminating beam. We found that during the very early stages of phase separation the SF scales with the wave vector q according to the Lorentzian q(-2), which shows that the liquid and vapor domains are just emerging. The critical wave number, which is related to the characteristic length of fluctuations, steadily decreases over time, supporting a sustained increase in the spatial scale of the fluctuating domains. The scaled evolution of the critical wave number obeys the universal evolution for the interconnected domains at high volume fraction with an apparent power law exponent of -0.35 ± 0.02. We also determined the correlation time of the fluctuations and inferred values for thermal diffusivity coefficient very near the critical point, above and below. The values were used to pinpoint the crossing of T(c) within 13 μK.
We report quantitative experimental results regarding concentration fluctuations based on a small-angle light-scattering setup. A shadowgraph technique was used to record concentration fluctuations in a free-diffusion cell filled with colloids. Our experimental setup includes an objective attached to the CCD camera to increase the field of view. We performed two separate experiments, one with 20 nm gold and the other with 200 nm silica colloids, and extracted both the structure factors and the correlation time during the early stages of concentration fluctuations. The temporal evolution of fluctuations was also qualitatively investigated using recursive plots and spatial-temporal sections of fluctuating images. We found that the correlation time versus wavenumber for gold nanocolloids is concave shaped, whereas, for silica colloids, it is convex shaped. The difference in correlation time behavior is not only due to the size of the particle, but also to possible plasmonic interactions in gold colloids.
By performing near-critical fluid experiments in the weightlessness of an orbiting space vehicle, we have suppressed buoyancy-driven flows and gravitational constraints on the liquid-gas interface of a large gas bubble. At equilibrium, the liquid completely wets the walls of a cylindrical cell, and the bubble is pushed to the sidewall. In these experiments the system's temperature T is increased at a constant rate past the critical temperature T(C), pushing it slightly out of equilibrium. The wetting film shows a large mechanical response to this heating, including contact lines that recede on a solid surface and a spreading bubble. Near T(C), the receding contact lines make the entire bubble appear to spread along the copper sidewall. The spreading bubble is a manifestation of the boiling crisis near the critical point. We present quantitative data of the receding contact lines that are observed prior to the near-critical boiling crisis. We analyze the receding contact lines in detail, and find that they are driven by vapor recoil from evaporation, as is the spreading bubble of the boiling crisis.
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