Observations of Dense Liquid Phase-Assisted Nanocrystal Growth and Coalescence

Author(s):  
Gen Li ◽  
Nana He ◽  
Junxian Deng ◽  
Jiaxin Liu ◽  
Yue Sun ◽  
...  
2017 ◽  
Vol 114 (38) ◽  
pp. E7882-E7890 ◽  
Author(s):  
Paul J. M. Smeets ◽  
Aaron R. Finney ◽  
Wouter J. E. M. Habraken ◽  
Fabio Nudelman ◽  
Heiner Friedrich ◽  
...  

Understanding and controlling nucleation is important for many crystallization applications. Calcium carbonate (CaCO3) is often used as a model system to investigate nucleation mechanisms. Despite its great importance in geology, biology, and many industrial applications, CaCO3nucleation is still a topic of intense discussion, with new pathways for its growth from ions in solution proposed in recent years. These new pathways include the so-called nonclassical nucleation mechanism via the assembly of thermodynamically stable prenucleation clusters, as well as the formation of a dense liquid precursor phase via liquid–liquid phase separation. Here, we present results from a combined experimental and computational investigation on the precipitation of CaCO3in dilute aqueous solutions. We propose that a dense liquid phase (containing 4–7 H2O per CaCO3unit) forms in supersaturated solutions through the association of ions and ion pairs without significant participation of larger ion clusters. This liquid acts as the precursor for the formation of solid CaCO3in the form of vaterite, which grows via a net transfer of ions from solution according tozCa2++zCO32−→zCaCO3. The results show that all steps in this process can be explained according to classical concepts of crystal nucleation and growth, and that long-standing physical concepts of nucleation can describe multistep, multiphase growth mechanisms.


2019 ◽  
Author(s):  
Naor Granik ◽  
Noa Katz ◽  
Sarah Goldberg ◽  
Roee Amit

AbstractObservations of liquid-liquid phase-separated compartments within living cells have generated important insights on intracellular processes in recent years. Here, we use PP7-coat protein and Qβ-coat protein together with multi-binding-site RNA scaffolds to generate synthetic phase-separated biocondensates within E. coli cells. Real-time tracking of entry and shedding of RNA-protein complexes into and out of the biocondensates reveals that the cytosol is divided into a dense liquid phase in the nucleoid-dominated region, and a dilute liquid phase in the polar regions. We provide evidence for this assertion using stationary phase cells, where emergence of non-polar biocondensate formation is consistent with a reduction in size of the dense-nucleoid phase. The bi-phasic hypothesis for the E.coli cytosol has implications for various transcriptional and translational processes, and could provide an alternative explanation for the Super-Poisson dynamics attributed to transcriptional bursts.One Sentence SummaryUsing synthetic liquid-liquid phase-separated biocondensates, we show that the E.coli’s cytosol is likely composed of a dense and dilute liquid phases.


Science ◽  
2013 ◽  
Vol 341 (6148) ◽  
pp. 885-889 ◽  
Author(s):  
Adam F. Wallace ◽  
Lester O. Hedges ◽  
Alejandro Fernandez-Martinez ◽  
Paolo Raiteri ◽  
Julian D. Gale ◽  
...  

Recent experimental observations of the onset of calcium carbonate (CaCO3) mineralization suggest the emergence of a population of clusters that are stable rather than unstable as predicted by classical nucleation theory. This study uses molecular dynamics simulations to probe the structure, dynamics, and energetics of hydrated CaCO3 clusters and lattice gas simulations to explore the behavior of cluster populations before nucleation. Our results predict formation of a dense liquid phase through liquid-liquid separation within the concentration range in which clusters are observed. Coalescence and solidification of nanoscale droplets results in formation of a solid phase, the structure of which is consistent with amorphous CaCO3. The presence of a liquid-liquid binodal enables a diverse set of experimental observations to be reconciled within the context of established phase-separation mechanisms.


2020 ◽  
Vol 117 (52) ◽  
pp. 33254-33262
Author(s):  
Maarten Hardenberg ◽  
Attila Horvath ◽  
Viktor Ambrus ◽  
Monika Fuxreiter ◽  
Michele Vendruscolo

A wide range of proteins have been reported to condensate into a dense liquid phase, forming a reversible droplet state. Failure in the control of the droplet state can lead to the formation of the more stable amyloid state, which is often disease-related. These observations prompt the question of how many proteins can undergo liquid–liquid phase separation. Here, in order to address this problem, we discuss the biophysical principles underlying the droplet state of proteins by analyzing current evidence for droplet-driver and droplet-client proteins. Based on the concept that the droplet state is stabilized by the large conformational entropy associated with nonspecific side-chain interactions, we develop the FuzDrop method to predict droplet-promoting regions and proteins, which can spontaneously phase separate. We use this approach to carry out a proteome-level study to rank proteins according to their propensity to form the droplet state, spontaneously or via partner interactions. Our results lead to the conclusion that the droplet state could be, at least transiently, accessible to most proteins under conditions found in the cellular environment.


Author(s):  
N.V. Belov ◽  
U.I. Papiashwili ◽  
B.E. Yudovich

It has been almost universally adopted that dissolution of solids proceeds with development of uniform, continuous frontiers of reaction.However this point of view is doubtful / 1 /. E.g. we have proved the active role of the block (grain) boundaries in the main phases of cement, these boundaries being the areas of hydrate phases' nucleation / 2 /. It has brought to the supposition that the dissolution frontier of cement particles in water is discrete. It seems also probable that the dissolution proceeds through the channels, which serve both for the liquid phase movement and for the drainage of the incongruant solution products. These channels can be appeared along the block boundaries.In order to demonsrate it, we have offered the method of phase-contrast impregnation of the hardened cement paste with the solution of methyl metacrylahe and benzoyl peroxide. The viscosity of this solution is equal to that of water.


Author(s):  
C.D. Humphrey ◽  
T.L. Cromeans ◽  
E.H. Cook ◽  
D.W. Bradley

There is a variety of methods available for the rapid detection and identification of viruses by electron microscopy as described in several reviews. The predominant techniques are classified as direct electron microscopy (DEM), immune electron microscopy (IEM), liquid phase immune electron microscopy (LPIEM) and solid phase immune electron microscopy (SPIEM). Each technique has inherent strengths and weaknesses. However, in recent years, the most progress for identifying viruses has been realized by the utilization of SPIEM.


Author(s):  
Michael P. Mallamaci ◽  
James Bentley ◽  
C. Barry Carter

Glass-oxide interfaces play important roles in developing the properties of liquid-phase sintered ceramics and glass-ceramic materials. Deposition of glasses in thin-film form on oxide substrates is a potential way to determine the properties of such interfaces directly. Pulsed-laser deposition (PLD) has been successful in growing stoichiometric thin films of multicomponent oxides. Since traditional glasses are multicomponent oxides, there is the potential for PLD to provide a unique method for growing amorphous coatings on ceramics with precise control of the glass composition. Deposition of an anorthite-based (CaAl2Si2O8) glass on single-crystal α-Al2O3 was chosen as a model system to explore the feasibility of PLD for growing glass layers, since anorthite-based glass films are commonly found in the grain boundaries and triple junctions of liquid-phase sintered α-Al2O3 ceramics.Single-crystal (0001) α-Al2O3 substrates in pre-thinned form were used for film depositions. Prethinned substrates were prepared by polishing the side intended for deposition, then dimpling and polishing the opposite side, and finally ion-milling to perforation.


Author(s):  
J. Drennan ◽  
R.H.J. Hannink ◽  
D.R. Clarke ◽  
T.M. Shaw

Magnesia partially stabilised zirconia (Mg-PSZ) ceramics are renowned for their excellent nechanical properties. These are effected by processing conditions and purity of starting materials. It has been previously shown that small additions of strontia (SrO) have the effect of removing the major contaminant, silica (SiO2).The mechanism by which this occurs is not fully understood but the strontia appears to form a very mobile liquid phase at the grain boundaries. As the sintering reaches the final stages the liquid phase is expelled to the surface of the ceramic. A series of experiments, to examine the behaviour of the liquid grain boundary phase, were designed to produce compositional gradients across the ceramic bodies. To achieve this, changes in both silica content and furnace atmosphere were implemented. Analytical electron microscope techniques were used to monitor the form and composition of the phases developed. This paper describes the results of our investigation and the presentation will discuss the work with reference to liquid phase sintering of ceramics in general.


Author(s):  
Mahesh Chandramouli

Magnetization reversal in sintered Fe-Nd-B, a complex, multiphase material, occurs by nucleation and growth of reverse domains making the isolation of the ferromagnetic Fe14Nd2B grains by other nonmagnetic phases crucial. The magnets used in this study were slightly rich in Nd (in comparison to Fe14Nd2B) to promote the formation of Nd-oxides at multigrain junctions and incorporated Dy80Al20 as a liquid phase sintering addition. Dy has been shown to increase the domain wall energy thus making nucleation more difficult while Al is thought to improve the wettability of the Nd-oxide phases.Bulk polished samples were examined in a JEOL 35CF scanning electron microscope (SEM) operated at 30keV equipped with a Be window energy dispersive spectrometer (EDS) detector in order to determine the phase distribution.


Author(s):  
N.A. Bert ◽  
A.O. Kosogov

The very thin (<100 Å) InGaAsP layers were grown not only by molecular beam epitaxy and metal-organic chemical vapor deposition but recently also by simple liquid phase epitaxy (LPE) technique. Characterization of their thickness, interfase abruptness and lattice defects is important and requires TEM methods to be used.The samples were InGaAsP/InGaP double heterostructures grown on (111)A GaAs substrate. The exact growth conditions are described in Ref.1. The salient points are that the quarternary layers were being grown at 750°C during a fast movement of substrate and a convection caused in the melt by that movement was eliminated. TEM cross-section specimens were prepared by means of conventional procedure. The studies were conducted in EM 420T and JEM 4000EX instruments.The (200) dark-field cross-sectional imaging is the most appropriate TEM technique to distinguish between individual layers in 111-v semiconductor heterostructures.


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