The microscopic kinetics of ubiquitous solid-solid phase transitions remain poorly understood. Here, by using single-particle-resolution video microscopy of colloidal films of diameter-tunable microspheres, we show that transitions between square and triangular lattices occur via a two-step diffusive nucleation pathway involving liquid nuclei. The nucleation pathway is favoured over the direct one-step nucleation because the energy of the solid/liquid interface is lower than that between solid phases. We also observed that nucleation precursors are particle-swapping loops rather than newly generated structural defects, and that coherent and incoherent facets of the evolving nuclei exhibit different energies and growth rates that can markedly alter the nucleation kinetics. Our findings suggest that an intermediate liquid should exist in the nucleation processes of solid-solid transitions of most metals and alloys, and provide guidance for better control of the kinetics of the transition and for future refinements of solid-solid transition theory.
We observed a two-step glass transition in monolayers of colloidal ellipsoids by video microscopy. The glass transition in the rotational degree of freedom was at a lower density than that in the translational degree of freedom. Between the two transitions, ellipsoids formed an orientational glass. Approaching the respective glass transitions, the rotational and translational fastest-moving particles in the supercooled liquid moved cooperatively and formed clusters with power-law size distributions. The mean cluster sizes diverge in power law as approaching the glass transitions. The clusters of translational and rotational fastest-moving ellipsoids formed mainly within pseudonematic domains, and around the domain boundaries, respectively. Colloids are outstanding model systems for glass transition studies because the trajectories of individual particles are measurable by video microscopy [1]. In the past two decades, significant experimental effort has been applied to studying colloidal glasses consisting of isotropic particles [1][2][3][4][5], but little to anisotropic particles [6]. The glass transition of anisotropic particles has been studied in three dimensions (3D) mainly through simulation [7,8]. Molecular mode-coupling theory (MMCT) predicts that particle anisotropy should lead to new phenomena in glass transitions [9,10], and some of these have been observed in recent 3D simulations of hard ellipsoids [11,12]. MMCT [10,13] suggests that hard ellipsoids with an aspect ratio p > 2.5 in 3D can form an orientational glass in which rotational degrees of freedom become glass while the center-of-mass motion remains ergodic [9]. Such a "liquid glass" [14], in analogy to a liquid crystal, has not yet been explored in 3D or even 2D experiments. Anisotropic particles should also enable exploration of the dynamic heterogeneity in the rotational degrees of freedom. Moreover the glass transitions of monodispersed particles have not yet been studied in 2D. It is well known that monodispersed spheres can be quenched to a glass in 3D, but hardly in 2D even at the fastest accessible quenching rate. Hence bidispersed or highly polydispersed spheres have been used in experiments [5,15,16], simulations [17] and theory [18] for 2D glasses. In contrast, we found that monodispersed ellipsoids of intermediate aspect ratio are excellent glass formers in 2D because their shape can effectively frustrate crystallization and nematic order.Here we investigate the glass transition in monolayers of colloidal ellipsoids using video microscopy. We measured the translational and rotational relaxation times, the non-Gaussian parameter of the distribution of displacements, and the clusters of cooperative fastestmoving particles. These results consistently showed that the glass transitions of rotational and translational motions occur in two different area fractions, defining an intermediate orientational glass phase.The ellipsoids were synthesized by stretching polymethyl methacrylate (PMMA) spheres [19,20]. They had a small polydispersity...
The nucleation process is crucial to many phase transitions, but its kinetics are difficult to predict and measure. We superheated and melted the interior of thermal-sensitive colloidal crystals and investigated by means of video microscopy the homogeneous melting at single-particle resolution. The observed nucleation precursor was local particle-exchange loops surrounded by particles with large displacement amplitudes rather than any defects. The critical size, incubation time, and shape and size evolutions of the nucleus were measured. They deviate from the classical nucleation theory under strong superheating, mainly because of the coalescence of nuclei. The superheat limit agrees with the measured Born and Lindemann instabilities.
When a liquid is supercooled towards the glass transition, its dynamics drastically slows down, whereas its static structure remains relatively unchanged. Finding a structural signature of the dynamic slowing down is a major challenge, yet it is often too subtle to be uncovered. Here we discover the structural signatures for both translational and rotational dynamics in monolayers of colloidal ellipsoids by video microscopy experiments and computer simulations. The correlation lengths of the dynamic slowest-moving clusters, the static glassy clusters, the static local structural entropy and the dynamic heterogeneity follow the same power-law divergence, suggesting that the kinetic slowing down is caused by a decrease in the structural entropy and an increase in the size of the glassy cluster. Ellipsoids with different aspect ratios exhibit single- or double-step glass transitions with distinct dynamic heterogeneities. These findings demonstrate that the particle shape anisotropy has important effects on the structure and dynamics of the glass.
Growth factors such as hepatocyte growth factor (HGF) are highly up-regulated during development and following renal injury and are known to induce marked morphogenic actions in cultured tubular epithelial cells, including scattering, migration, single cell branching morphogenesis, and multicellular branching tubulogenesis. In the present study, we demonstrate that HGF stimulates epithelial cells to express neutrophil gelatinase-associated lipocalin (Ngal), a member of the lipocalin family of secreted proteins that has recently been shown to participate in mesenchymal-epithelial transformation via its ability to augment cellular iron uptake. At concentrations below those found to mediate iron transport, purified Ngal can induce a promigratory and probranching effect that is dependent on ERK activation. The suppression of Ngal expression using short hairpin RNA results in increased cyst formation by tubular cells. However, the simultaneous addition of Ngal and HGF leads to direct association of the two proteins, and results in a partial inhibition of HGF-mediated activation of c-Met and the downstream MAPK and phosphatidylinositol 3-kinase signaling pathways. This inhibitory effect down-regulates HGF-stimulated single cell migration, and limits branching morphogenesis at both the single cell and multicellular level. These experiments demonstrate that the local expression of Ngal can play a regulatory role in epithelial morphogenesis by promoting the organization of cells into tubular structures while simultaneously negatively modulating the branching effects of HGF.
Crystal surfaces typically melt into a thin liquid layer at temperatures slightly below the melting point of the crystal. Such surface premelting is prevalent in all classes of solids and is important in a variety of metallurgical, geological and meteorological phenomena. Premelting has been studied using X-ray diffraction and differential scanning calorimetry, but the lack of single-particle resolution makes it hard to elucidate the underlying mechanisms. Colloids are good model systems for studying phase transitions because the thermal motions of individual micrometre-sized particles can be tracked directly using optical microscopy. Here we use colloidal spheres with tunable attractions to form equilibrium crystal-vapour interfaces, and study their surface premelting behaviour at the single-particle level. We find that monolayer colloidal crystals exhibit incomplete premelting at their perimeter, with a constant liquid-layer thickness. In contrast, two- and three-layer crystals exhibit conventional complete melting, with the thickness of the surface liquid diverging as the melting point is approached. The microstructures of the surface liquids differ in certain aspects from what would be predicted by conventional premelting theories. Incomplete premelting in the monolayer crystals is triggered by a bulk isostructural solid-solid transition and truncated by a mechanical instability that separately induces homogeneous melting within the bulk. This finding is in contrast to the conventional assumption that two-dimensional crystals melt heterogeneously from their free surfaces (that is, at the solid-vapour interface). The unexpected bulk melting that we observe for the monolayer crystals is accompanied by the formation of grain boundaries, which supports a previously proposed grain-boundary-mediated two-dimensional melting theory. The observed interplay between surface premelting, bulk melting and solid-solid transitions challenges existing theories of surface premelting and two-dimensional melting.
Solid–solid transitions between crystals follow diffusive nucleation, or various diffusionless transitions, but these kinetics are difficult to predict and observe. Here we observed the rich kinetics of transitions from square lattices to triangular lattices in tunable colloidal thin films with single-particle dynamics by video microscopy. Applying a small pressure gradient in defect-free regions or near dislocations markedly transform the diffusive nucleation with an intermediate-stage liquid into a martensitic generation and oscillation of dislocation pairs followed by a diffusive nucleus growth. This transformation is neither purely diffusive nor purely martensitic as conventionally assumed but a combination thereof, and thus presents new challenges to both theory and the empirical criterion of martensitic transformations. We studied how pressure, density, grain boundary, triple junction and interface coherency affect the nucleus growth, shape and kinetic pathways. These novel microscopic kinetics cast new light on control solid–solid transitions and microstructural evolutions in polycrystals.
The growth behaviour of liquid nucleus is crucial for crystal melting, but its kinetics is difficult to predict and remains challenging in experiment. Here we directly observed the growth of individual liquid nuclei in homogeneous melting of three-dimensional superheated colloidal crystals with single-particle dynamics by video microscopy. The growth rate of nucleus at weak superheating is well fitted by generalizing the Wilson–Frenkel law of crystallization to melting and including the surface tension effects and non-spherical-shape effects. As the degree of superheating increases, the growth rate is enhanced by nucleus shape fluctuation, nuclei coalescence and multimer attachment. The results provide new guidance for the refinement of nucleation theory, especially for the poorly understood strong-superheating regime. The universal Lindemann parameter observed at the superheat limit and solid–liquid interfaces indicates a connection between homogeneous and heterogeneous melting.
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