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Register a new userHydrodynamic coarsening in phase-separated silicate melts
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Added by
Emmanuelle Gouillart
Publication date
2015
fields
Physics
and research's language is
English
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Using in-situ synchrotron tomography, we investigate the coarsening dynamics of barium borosilicate melts during phase separation. The 3-D geometry of the two interconnected phases is determined thanks to image processing. We observe a linear growth of the size of domains with time, at odds with the sublinear diffusive growth usually observed in phase-separating glasses or alloys. Such linear coarsening is attributed to viscous flow inside the bicontinuous phases, and quantitative measurements show that the growth rate is well explained by the ratio of surface tension over viscosity. The geometry of the domains is shown to be statistically similar at different times, provided that the microstructure is rescaled by the average domain size. Complementary experiments on melts with a droplet morphology demonstrate that viscous flow prevails over diffusion in the large range of domain sizes measured in our experiments (1 - 80 microns).
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Coarsening kinetics is usually described using a linear gradient approximation for the underlying interface migration (IM) rates, wherein the migration fluxes at the interfaces vary linearly with the driving force. Recent experimental studies have shown that coarsening of nanocrystalline interface microstructures is unexpectedly stable compared to conventional parabolic coarsening kinetics. Here, we show that during early stage coarsening of these microstructures, IM rates can develop a non-linear dependence on the driving force, the mean interface curvature. We derive the modified mean field law for coarsening kinetics. Molecular dynamics simulations of individual grain boundaries reveal a sub-linear curvature dependence of IM rates, suggesting an intrinsic origin for the slow coarsening kinetics observed in polycrystalline metals.
We have studied the irreversibility of the magnetization induced by thermal cycles in La0.5Ca0.5MnO3 manganites, which present a low temperature state characterized by the coexistence of phases. The effect is evidenced by a decrease of the magnetization after cycling the sample between 300 and 50 K. We developed a phenomenological model that allows us to correlate the value of the magnetization with the number of cycles performed. The experimental results show excellent agreement with our model, suggesting that this material could be used for the development of a device to monitor thermal changes. The effect of thermal cycling is towards an increase of the amount of the non ferromagnetic phase in the compounds and it might be directly related with the strain at the contact surface among the coexisting phases.
We have studied magnetic and transport properties on different manganese oxide based compounds exhibiting phase separation: polycrystalline La5/8-yPryCa3/8MnO3 (y=0.3) and La1/2Ca1/2Mn1-zFezO3 (z = 0.05), and single crystals of La5/8-yPryCa3/8MnO3 (y=0.35). Time dependent effects indicate that the fractions of the coexisting phases are dynamically changing in a definite temperature range. We found that in this range the ferromagnetic fraction f can be easily tuned by application of low magnetic fields (< 1 T). The effect is persistent after the field is turned off, thus the field remains imprinted in the actual value of f and can be recovered through transport measurements. This effect is due both to the existence of a true phase separated equilibrium state with definite equilibrium fraction f0, and to the slow growth dynamics. The fact that the same global features were found on different compounds and in polycrystalline and single crystalline samples, suggests that the effect is a general feature of some phase separated media.
We review a few representative examples of granular experiments or models where phase separation, accompanied by domain coarsening, is a relevant phenomenon. We first elucidate the intrinsic non-equilibrium, or athermal, nature of granular media. Thereafter, dilute systems, the so-called granular gases are discussed: idealized kinetic models, such as the gas of inelastic hard spheres in the cooling regime, are the optimal playground to study the slow growth of correlated structures, e.g. shear patterns, vortices and clusters. In fluidized experiments, liquid-gas or solid-gas separations have been observed. In the case of monolayers of particles, phase coexistence and coarsening appear in several different setups, with mechanical or electrostatic energy input. Phenomenological models describe, even quantitatively, several experimental measures, both for the coarsening dynamics and for the dynamic transition between different granular phases. The origin of the underlying bistability is in general related to negative compressibility from granular hydrodynamics computations, even if the understanding of the mechanism is far from complete. A relevant problem, with important industrial applications, is related to the demixing or segregation of mixtures, for instance in rotating tumblers or on horizontally vibrated plates. Finally, the problem of compaction of highly dense granular materials, which has many important applications, is usually described in terms of coarsening dynamics: there, bubbles of mis-aligned grains evaporate, allowing the coalescence of optimally arranged islands and a progressive reduction of total occupied volume.
We have investigated the change in entropy with direct measurements of heat flow as a function of magnetic field at fixed temperatures across the entire phase diagram of the phase-separated (PS) compound La$_{0.25}$Pr$_{0.375}$Ca$_{0.375}$MnO$_3$ (LPCMO). At this composition, the compound shows competing charge-ordered/antiferromagnetic (CO/AF) ground states. At a fixed temperature, we observe an increase in hysteresis in the entropy as a function of the applied field. The heat flux shows progressively irreversible hysteresis, which characterizes the energy barriers between the two competing ground states, as the temperature is lowered. The increase in the heat loss correlates with the increase in magnetic viscosity in the phase-separated state. Keywords: manganites, avalanche effect, phase transition, heat flow, DSC, entropy. Corresponding author: [email protected] . On 10 April 2020, this JAC-Elsevier article was accepted. Yet, its online publication shows numerous errors: Cut-off text, missing Figure Captions, incomplete Table ... None of which is our fault! This makes our paper hard to read, study and/or understand. This reproduction is our final (error-free!) revision. When citing our refereed paper, please also refer to this arXiv print. Thank you for understanding
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