Crystal nucleation in glass-forming liquids: Variation of the size of the “structural units” with temperature

Fokin, Vladimir M.; Abyzov, Alexander S.; Zanotto, Edgar Dutra; Cassar, Daniel R.; Rodrigues, Alisson Mendes; Schmelzer, Jürn W. P.

doi:10.1016/j.jnoncrysol.2016.05.017

Cited by 61 publications

(84 citation statements)

References 36 publications

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“…Performing measurements of the steady‐state nucleation rates and the time lag in nucleation, a combination of Eqs. and allows one to eliminate the kinetic coefficients and to determine the work of critical cluster formation in dependence on temperature based on experimental data . A typical result is shown in Fig.…”

Section: Thermodynamic Driving Force Specific Surface Energy and Womentioning

confidence: 98%

“…These curves have been calculated from measured nucleation rates and induction times as reported in (cf. also).…”

Section: Thermodynamic Driving Force Specific Surface Energy and Womentioning

confidence: 99%

“…An interpretation of the minimum of the work of critical cluster formation employing appropriate dependencies d = d ( T ) is given in . The interpretation of this dependence in terms of more correct kinetic models is sketched there as well.…”

Section: Thermodynamic Driving Force Specific Surface Energy and Womentioning

confidence: 99%

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Crystallization of Glass: What We Know, What We Need to Know

Schmelzer

Fokin

Abyzov

2016

Int J of Appl Glass Sci

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The relevance of the concepts of fragility and of the glass transition temperature for the understanding of crystal nucleation and growth in glass-forming liquids is explored. It is shown that classical fragility can be relevant for the understanding of the crystallization behavior only if several severe conditions are fulfilled that are rarely met. By this reason, a new definition of liquid fragility is introduced shown to be able to reflect appropriately the maxima of crystal nucleation, growth, and overall crystallization rates. The origin of the previously reported correlations between glass transition temperatures and intensity of crystallization processes is specified. Further, interpreted in terms of classical nucleation theory, for a variety of oxide glassforming liquids, the thermodynamic barrier for homogeneous crystal nucleation exhibits at high undercooling an unusual increase with a decrease in temperature. Such behavior cannot be explained in terms of classical nucleation theory. Different directions of generalization of the classical theory are discussed, which may lead to a resolution of these problems. The realization of such generalization is considered to be a prerequisite for a generally deeper understanding of the complex phenomena occurring in melt crystallization with its rich field of applications.

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Section: Thermodynamic Driving Force Specific Surface Energy and Womentioning

confidence: 98%

“…These curves have been calculated from measured nucleation rates and induction times as reported in (cf. also).…”

Section: Thermodynamic Driving Force Specific Surface Energy and Womentioning

confidence: 99%

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Crystallization of Glass: What We Know, What We Need to Know

Schmelzer

Fokin

Abyzov

2016

Int J of Appl Glass Sci

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“… (a) : N ( t )/( J ( T ) τ ) versus reduced time, t / τ , for glasses Li

_{2}

O · 2SiO

_{2}

(1)–(2) and 2Na

_{2}

O · CaO · 3SiO

_{2}

(3) – (4) for T = 430 (1) , 465 (2) , 465 (3) , and

470^{o}

C (4) . (b) : Reduced nucleation rate, J ( t , T )/ J ( T ), versus reduced time, t / τ …”

Section: Characteristic Time‐scales In Nucleation: Isothermal and Isomentioning

confidence: 99%

“…. The values of the time‐lags employed are included and are denoted as

τ_{S}

(Shneidman) and

τ_{K}

(Collins–Kashchiev), respectively …”

Section: Characteristic Time‐scales In Nucleation: Isothermal and Isomentioning

confidence: 99%

Time of Formation of the First Supercritical Nucleus, Time‐lag, and the Steady‐State Nucleation Rate

Schmelzer

Abyzov

Байдаков

2016

Int J of Appl Glass Sci

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General equations are derived for the description of correlations between average time of formation of the first supercritical nucleus, time‐lag in nucleation, and steady‐state nucleation rate. In their implementation, a set of representative equations is employed modeling the time‐dependence of the nucleation rate as proposed first by Zeldovich and advanced by a variety of other authors. The analysis is performed for both isothermal–isobaric and time‐dependent process conditions. It is shown that, in general, the time of formation of the first supercritical nucleus depends both on time‐lag and the average time of formation of a supercritical nucleus at steady‐state conditions. The conditions are specified at which one of these characteristic times may dominate. In contrast to alternative statements it is also demonstrated that for isothermal–isobaric conditions, due to the Poisson character of nucleation, steady‐state nucleation rates can be determined without having at one's disposal a detailed knowledge of the time‐lag and the kinetic laws of approach of steady‐state nucleation conditions. Results of molecular‐dynamics simulations of crystal nucleation in Lennard‐Jones liquids are presented for an illustration of the general conclusions. Several applications of the results to the interpretation of experimental data are discussed.

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2019

Glass‐Ceramic Technology

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Crystal nucleation in glass-forming liquids: Variation of the size of the “structural units” with temperature

Cited by 61 publications

References 36 publications

Crystallization of Glass: What We Know, What We Need to Know

Crystallization of Glass: What We Know, What We Need to Know

Time of Formation of the First Supercritical Nucleus, Time‐lag, and the Steady‐State Nucleation Rate

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