Imaging the Homogeneous Nucleation During the Melting of Superheated Colloidal Crystals

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.

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Homogeneous nucleation of n-nonane and n-propanol mixtures: A comparison of classical nucleation theory and experiments

The Journal of Chemical Physics ◽

10.1063/1.2138703 ◽

2005 ◽

Vol 123 (24) ◽

pp. 244502 ◽

Cited By ~ 20

Author(s):

A. I. Gaman ◽

I. Napari ◽

P. M. Winkler ◽

H. Vehkamäki ◽

P. E. Wagner ◽

...

Keyword(s):

Homogeneous Nucleation ◽

Nucleation Theory ◽

Classical Nucleation Theory ◽

Theory And Experiments

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Analytical Investigation on the Homogeneous Nucleation in a Mono-Component and Bi-Component Droplet

ASME 2019 6th International Conference on Micro/Nanoscale Heat and Mass Transfer ◽

10.1115/mnhmt2019-3968 ◽

2019 ◽

Author(s):

Xi Xi ◽

Hong Liu ◽

Chang Cai ◽

Ming Jia ◽

Weilong Zhang

Keyword(s):

Nucleation Rate ◽

Homogeneous Nucleation ◽

Ambient Pressure ◽

Analytical Investigation ◽

Bubble Nucleation ◽

Nucleation Theory ◽

Classical Nucleation Theory ◽

Liquid Temperature ◽

Wide Range ◽

Good Agreement

Abstract The work attempts to analyze the performance of homogeneous nucleation by using the non-equilibrium thermodynamics theory and the classical nucleation theory. A nucleation rate graph was constructed under a wide range of operating temperature conditions. The results indicate that the superheat limit temperature (SLT) estimated by the modified homogeneous nucleation sub-model is in good agreement with the experimental results. The nucleation rate increases exponentially with the liquid temperature rise when the liquid temperature exceeds the SLT under atmospheric pressure. The superheated temperature needed to trigger the bubble nucleation decreases with the elevated ambient pressure.

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Molecular Dynamics Based Analysis of Nucleation and Surface Energy of Droplets in Supersaturated Vapors of Methane and Ethane

Journal of Heat Transfer ◽

10.1115/1.3072909 ◽

2009 ◽

Vol 131 (4) ◽

Cited By ~ 10

Author(s):

Jadran Vrabec ◽

Martin Horsch ◽

Hans Hasse

Keyword(s):

Molecular Dynamics ◽

Surface Energy ◽

Droplet Size ◽

Nucleation Rate ◽

Homogeneous Nucleation ◽

First Passage Time ◽

Nucleation Theory ◽

Dynamics Simulation ◽

Classical Nucleation Theory ◽

Critical Droplet

Homogeneous nucleation processes are characterized by the nucleation rate and the critical droplet size. Molecular dynamics simulation is applied for studying homogeneous nucleation during condensation of supersaturated vapors of methane and ethane. The results are compared with the classical nucleation theory (CNT) and the Laaksonen–Ford–Kulmala (LFK) model that introduces the size dependence of the specific surface energy. It is shown for the nucleation rate that the Yasuoka–Matsumoto method and the mean first passage time method lead to considerably differing results. Even more significant deviations are found between two other approaches to the critical droplet size, based on the maximum of the Gibbs free energy of droplet formation (Yasuoka–Matsumoto) and the supersaturation dependence of the nucleation rate (nucleation theorem). CNT is found to agree reasonably well with the simulation results, whereas LFK leads to large deviations at high temperatures.

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Direct calculation of ice homogeneous nucleation rate for a molecular model of water

Proceedings of the National Academy of Sciences ◽

10.1073/pnas.1509267112 ◽

2015 ◽

Vol 112 (34) ◽

pp. 10582-10588 ◽

Cited By ~ 135

Author(s):

Amir Haji-Akbari ◽

Pablo G. Debenedetti

Keyword(s):

Homogeneous Nucleation ◽

Molecular Model ◽

Direct Calculation ◽

Nucleation Theory ◽

Coarse Grained ◽

Classical Nucleation Theory ◽

Molecular Models ◽

Microscopic Mechanism ◽

Hexagonal Ice ◽

Ice Leads

Ice formation is ubiquitous in nature, with important consequences in a variety of environments, including biological cells, soil, aircraft, transportation infrastructure, and atmospheric clouds. However, its intrinsic kinetics and microscopic mechanism are difficult to discern with current experiments. Molecular simulations of ice nucleation are also challenging, and direct rate calculations have only been performed for coarse-grained models of water. For molecular models, only indirect estimates have been obtained, e.g., by assuming the validity of classical nucleation theory. We use a path sampling approach to perform, to our knowledge, the first direct rate calculation of homogeneous nucleation of ice in a molecular model of water. We use TIP4P/Ice, the most accurate among existing molecular models for studying ice polymorphs. By using a novel topological approach to distinguish different polymorphs, we are able to identify a freezing mechanism that involves a competition between cubic and hexagonal ice in the early stages of nucleation. In this competition, the cubic polymorph takes over because the addition of new topological structural motifs consistent with cubic ice leads to the formation of more compact crystallites. This is not true for topological hexagonal motifs, which give rise to elongated crystallites that are not able to grow. This leads to transition states that are rich in cubic ice, and not the thermodynamically stable hexagonal polymorph. This mechanism provides a molecular explanation for the earlier experimental and computational observations of the preference for cubic ice in the literature.

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Predicting glass-to-glass and liquid-to-liquid phase transitions in supercooled water using classical nucleation theory

Chemical Physics ◽

10.1016/j.chemphys.2017.11.008 ◽

2018 ◽

Vol 500 ◽

pp. 45-53 ◽

Cited By ~ 5

Author(s):

Robert F. Tournier

Keyword(s):

Phase Transitions ◽

Liquid Phase ◽

Supercooled Water ◽

Nucleation Theory ◽

Classical Nucleation Theory

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Mechanistic inferences from analysis of measurements of protein phase transitions in live cells

10.1101/2020.11.04.369017 ◽

2020 ◽

Author(s):

Ammon E. Posey ◽

Kiersten M. Ruff ◽

Jared M. Lalmansingh ◽

Tejbir S. Kandola ◽

Jeffrey J. Lange ◽

...

Keyword(s):

Phase Transitions ◽

Phase Separation ◽

Phase Behavior ◽

Driving Forces ◽

Local Density ◽

Expression Profiles ◽

Resonance Energy ◽

Nucleation Theory ◽

Classical Nucleation Theory ◽

Live Cells

AbstractThe combination of phase separation and disorder-to-order transitions can give rise to ordered, semi-crystalline fibrillar assemblies that underlie prion phenomena namely, the non-Mendelian transfer of information across cells. Recently, a method known as Distributed Amphifluoric Förster Resonance Energy Transfer (DAmFRET) was developed to study the convolution of phase separation and disorder-to-order transitions in live cells. In this assay, a protein of interest is expressed to a broad range of concentrations and the acquisition of local density and order, measured by changes in FRET, is used to map phase transitions for different proteins. The high-throughput nature of this assay affords the promise of uncovering sequence-to-phase behavior relationships in live cells. Here, we report the development of a supervised method to obtain automated and accurate classifications of phase transitions quantified using the DAmFRET assay. Systems that we classify as undergoing two-state discontinuous transitions are consistent with prion-like behaviors, although the converse is not always true. We uncover well-established and surprising new sequence features that contribute to two-state phase behavior of prion-like domains. Additionally, our method enables quantitative, comparative assessments of sequence-specific driving forces for phase transitions in live cells. Finally, we demonstrate that a modest augmentation of DAmFRET measurements, specifically time-dependent protein expression profiles, can allow one to apply classical nucleation theory to extract sequence-specific lower bounds on the probability of nucleating ordered assemblies. Taken together, our approaches lead to a useful analysis pipeline that enables the extraction of mechanistic inferences regarding phase transitions in live cells.

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Homogeneous nucleation of NaCl in supersaturated solutions

Physical Chemistry Chemical Physics ◽

10.1039/d1cp02093e ◽

2021 ◽

Author(s):

Cintia Pulido Lamas ◽

Jorge R. Espinosa ◽

María Martín Conde ◽

Jorge Ramirez ◽

Pablo Montero de Hijes ◽

...

Keyword(s):

Molecular Dynamics ◽

Molecular Dynamics Simulations ◽

Homogeneous Nucleation ◽

Nucleation Theory ◽

Classical Nucleation Theory ◽

Approximate Approach ◽

Seeding Method ◽

Dynamics Simulations ◽

Supersaturated Solutions

The Seeding method is an approximate approach to investigate nucleation that combines molecular dynamics simulations with classical nucleation theory. This technique has been successfully implemented in a broad range of...

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HOMOGENEOUS NUCLEATION OF ICE IN WATER AS A FUNCTION OF PRESSURE: A TEST OF CLASSICAL NUCLEATION THEORY

Collied and Interface Science ◽

10.1016/b978-0-12-404502-6.50006-8 ◽

1976 ◽

pp. 23-29 ◽

Cited By ~ 1

Author(s):

Charles A. Knight

Keyword(s):

Homogeneous Nucleation ◽

Nucleation Theory ◽

Classical Nucleation Theory

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Concluding remarks

Faraday Discussions ◽

10.1039/c5fd00042d ◽

2015 ◽

Vol 179 ◽

pp. 543-547 ◽

Cited By ~ 7

Author(s):

Allan S. Myerson

Keyword(s):

Crystallization Process ◽

Crystal Form ◽

Nucleation Theory ◽

Crystal Nucleation ◽

Classical Nucleation Theory ◽

Nucleation Process ◽

Nucleation Mechanisms ◽

Process Work ◽

And Control ◽

Crystallization From Solution

Crystallization from solution is a crucial process used in the manufacture of a wide variety of materials. The first step in the crystallization process is the birth of a new crystalline phase, which is known as nucleation. Nucleation plays a key role in determining the results of any crystallization process with respect to the size, shape and crystal form obtained. Classical nucleation theory does not adequately explain the crystal nucleation process. Work described in the literature and at this Faraday Discussion describe more complex nucleation mechanisms which are generally known as two-step nucleation models. In addition, as most nucleation is influenced by dust, dirt and container surfaces, the importance of heterogeneous nucleation and the use of templates to accelerate nucleation and influence crystal form are promising methods for the study and control of nucleation. It is also clear from this Faraday Discussion that interest in this topic has grown, and new and novel experimental and modeling approaches are being used for the study of crystal nucleation from solution.

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