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1.
Инвентарный номер: нет.
   
   S 34


    Schmelzer, J. W. P.
    Classical and generalized Gibbs' approaches and the work of critical cluster formation in nucleation theory [Electronic resource] / J. W. P. Schmelzer, G. Sh. Boltachev, V. G. Baidakov // Journal of Chemical Physics. - 2006. - Vol. 124, № 19. - P194503/1-194503/18
ББК 53
Рубрики: ФИЗИКА
Кл.слова (ненормированные):
CLUSTERS
Аннотация: In the theoretical interpretation of the kinetics of first-order phase transitions, thermodynamic concepts developed long ago by Gibbs are widely employed giving some basic qualitative insights into these processes. However, from a quantitative point of view, the results of such analysis, based on the classical Gibbs approach and involving in addition the capillarity approximation, are often not satisfactory. Some progress can be reached here by the van der Waals and more advanced density functional methods of description of thermodynamically heterogeneous systems having, however, its limitations in application to the interpretation of experimental data as well. Moreover, both mentioned theories—Gibbs’ and density functional approaches—lead to partly contradicting each other’s results. As shown in preceding papers, by generalizing Gibbs’ approach, existing deficiencies and internal contradictions of these two well-established theories can be removed and a new generally applicable tool for the interpretation of phase formation processes can be developed. In the present analysis, a comparative analysis of the basic assumptions and predictions of the classical and the generalized Gibbs approaches is given. It is shown, in particular, that—interpreted in terms of the generalized Gibbs approach—the critical cluster as determined via the classical Gibbs approach corresponds not to a saddle but to a ridge point of the appropriate thermodynamic potential hypersurface. By this reason, the classical Gibbs approach (involving the classical capillarity approximation) overestimates as a rule the work of critical cluster formation in nucleation theory and, in general, considerably.

\\\\Expert2\\NBO\\Journal of Chemical Physics\\2006, v.124, p.194503.pdf
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2.
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   S 34


    Schmelzer, J. W. P.
    Kinetics of Boiling in Binary Liquid-Gas Solutions : A New Approach / J. W. P. Schmelzer, V. G. Baidakov, G. Sh. Boltachev // Nucleation Theory and Applications. - Dubna : JINR, 2002. - С. 120-145. - Bibliogr. : p.140-145 (83 ref.)
ББК 53
Рубрики: ФИЗИКА
Кл.слова (ненормированные):
CLUSTERS -- LIQUIDS -- HOMOGENEOUS NUCLEATION

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3.
Инвентарный номер: нет.
   
   B 16


    Baidakov, V. G.
    Comparison of Different Approaches to the Determination of the Work of Critical Cluster Formation / V. G. Baidakov, G. Sh. Boltachev, J. W. P. Schmelzer // Journal of Colloid and Interface Sience. - 2000. - Vol. 231, № 2. - С. 312-321
ББК 53
Рубрики: ФИЗИКА
Кл.слова (ненормированные):
CRITICAL CLUSTER -- GIBBS' METHOD -- NUCLEATION RATES
Аннотация: A comparative analysis of the results of determination of the work of critical cluster formation in nucleation theory for three different methods of evaluation—Gibbs' method, the van der Waals-Cahn and Hilliard, and a newly developed modified Gibbs' approach—is given. As a model system for comparison, regular solutions are chosen. In addition to the work of critical cluster formation, the composition of the critical clusters, their characteristic sizes and the values of the surface tension are determined in dependence on the initial supersaturation in the system or, equivalently, on the size of the critical clusters. It is found, in particular, that, for regular solutions, Tolman's equation cannot serve as a first approximation for the description of the curvature dependence of the surface tension even for large cluster sizes and an alternative formula is developed. It is shown that the latter two mentioned methods of determination of the work of critical cluster formation (the van der Waals-Cahn and Hilliard and the modified Gibbs' approach) lead—at least for the model system considered—to qualitatively and partly quantitatively equivalent results. Nevertheless, differences remain which may lead to quantitative deviations when applied to the determination of the steady-state nucleation rates. The possible origin of such deviations is discussed and some further directions of analysis are anticipated

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4.
Инвентарный номер: нет.
   
   S 34


    Schmelzer, J. W. P.
    Comment on “Multicomponent nucleation: Thermodynamically consistent description of the nucleation work” / J. W. P. Schmelzer, V. G. Baidakov // Journal of Chemical Physics. - 2004. - Vol.121, №3. - С. 1644-1645
ББК 53
Рубрики: ФИЗИКА
Кл.слова (ненормированные):
THERMODYNAMICALLY CONSISTENT -- NUCLEATIONS -- CRITICAL CLUSTER
Аннотация: In the above cited paper, Kashchiev extends the “thermodynamically consistent” description of nucleation work to phase formation processes in multicomponent systems. It is claimed that this approach is generally applicable widely independent on the kind of phase transformation considered. In contrast to this statement, it is shown in our Comment that Kashchiev’s approach is theoretically not well founded. It contains, in addition, a number of assumptions, which are not generally fulfilled. Because of this his method cannot give, in general, a satisfactory determination of the work of critical cluster formation in nucleation theory. An experimental example is given verifying our

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5.
Инвентарный номер: нет.
   
   B 74


    Boltachev, G. Sh.
    First-order curvature corrections to the surface tension of multicomponent systems / G. Sh. Boltachev, J. W. P. Schmelzer, V. G. Baidakov // Journal of Colloid and Interface Sience. - 2003. - Vol.264, №1. - С. 228-236
ББК 53
Рубрики: ФИЗИКА
Кл.слова (ненормированные):
SURFACE TENSION -- PHASE COEXISTENCE -- MULTICOMPONENT SYSTEMS
Аннотация: The dependence of surface tension on curvature is investigated for the case of an equilibrium phase coexistence in multicomponent systems. Employing Gibbs's method of description of heterogeneous systems, an equation is derived to determine the dependence of surface tension on curvature for widely arbitrary paths of variation of the independent thermodynamic parameters. It is supposed hereby merely that the temperature is kept constant and that the variations of the different molar fractions are such that the radius of the dividing surface varies monotonically in dependence on the change of the state parameters of the ambient phase along any of the chosen paths. In the analysis, an approach developed by Blokhuis and Bedeaux for one-component systems is utilized. It relies on the expansion of the surface free energy on curvature of the dividing surface. An equation is derived that connects the first-order correction term in the expansion with the interaction potential of the particles in the multicomponent solution and with the two-particle distribution functions in the planar interfacial layer between the two phases coexisting in equilibrium at planar interfaces. The connection of the first-order curvature correction to the surface tension and the first moment of the pressure tensor at a planar interface is analyzed as well

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6.
Инвентарный номер: нет.
   
   S 34


    Schmelzer, J. W. P.
    On different possibilities of a thermodynamically consistent determination of the work of critical cluster formation in nucleation theory / J. W. P. Schmelzer, V. G. Baidakov // Journal of Chemical Physics. - 2003. - Vol.119, №20. - С. 10759-10763
ББК 53
Рубрики: ФИЗИКА
Кл.слова (ненормированные):
THERMODYNAMIC PROPERTIES -- CLUSTERS -- NUCLEATION
Аннотация: In a recent paper [J. Chem. Phys. 118, 1837 (2003)], Kashchiev claimed to have developed a general thermodynamically consistent formula allowing one to describe correctly the work of critical cluster formation in one-component systems for a variety of cases of formation of gaseous, liquid, and solid phases. It is shown that most of the consequences drawn lack any substantiation

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7.
Инвентарный номер: нет.
   
   S 34


    Schmelzer, J. W. P.
    Kinetics of boiling in binary liquid–gas solutions: Comparison of different approaches / J. W. P. Schmelzer, V. G. Baidakov, G. Sh. Boltachev // Journal of Chemical Physics. - 2003. - Vol.119, №12. - С. 6166-6183
ББК 53
Рубрики: ФИЗИКА
Кл.слова (ненормированные):
CRITICAL CLUSTER -- GIBBS' METHOD -- VAN-DER-WAALS
Аннотация: A comparative analysis of the results of determination of the work of critical cluster formation in nucleation theory for three different methods of evaluation—Gibbs’ method (employing the capillarity approximation), the van der Waals–Cahn and Hilliard and a newly developed modified Gibbs’ approach—is given in application to phase formation in multicomponent systems. As an example, processes of boiling in binary liquid–gas solutions, in particular, in nitrogen–helium mixtures are investigated. In addition to the work of critical cluster formation, the bulk properties of the critical bubbles, their characteristic sizes and the values of the surface tension are determined in dependence on the initial supersaturation in the system or, equivalently, on the size of the critical clusters. It is shown that latter two mentioned methods (the van der Waals–Cahn and Hilliard and the modified Gibbs’ approach) lead, in the determination of the work of critical cluster formation, to qualitatively and widely even quantitatively equivalent results. As one of the more general consequences from the present analysis, it has been proven that the modified Gibbs’ approach represents a highly effective tool for the determination of the work of formation of clusters or bubbles of critical sizes not only for one-component and quasibinary systems, discussed earlier, but for phase formation in multicomponent systems of, in general, arbitrary numbers of components as well. It is shown that the modified Gibbs’ approach is preferable as compared with Gibbs’ original treatment not only due to its advantages with respect to an appropriate determination of the properties of clusters of critical sizes, but also from general theoretical considerations. In the limit of large sizes of the critical clusters, both approaches—Gibbs’ original treatment and the modified or generalized Gibbs’ approach—lead to equivalent results

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8.
Инвентарный номер: нет.
   
   S 34


    Schmelzer, J. W. P.
    Kinetics of Condensation and Boiling: Comparison of Different Approaches / J. W. P. Schmelzer, V. G. Baidakov // Journal of Physical Chemistry B. - 2001. - Vol.105, №47. - С. 11595-11604
ББК 53
Рубрики: ФИЗИКА
Кл.слова (ненормированные):
CRITICAL CLUSTER -- GIBBS' METHOD -- VAN-DER-WAALS METHOD -- HILLIARD METHOD
Аннотация: A comparative analysis of the results of determination of the work of critical cluster formation in nucleation theory for three different methods of evaluationGibbs' method (employing the capillarity approximation), the van der Waals−Cahn and Hilliard method, and a newly developed modified Gibbs approachis given. As a particular application, the processes of condensation and boiling in one-component fluids are analyzed. As a model system for comparison, van der Waals fluids are chosen. In addition to the work of critical cluster formation, the bulk properties of the critical clusters (drops or bubbles), their characteristic sizes, and the values of the surface tension are determined in dependence on the initial supersaturation in the system or, equivalently, on the size of the critical clusters. It is shown that latter two mentioned methods of determination of the work of critical cluster formation (the van der Waals−Cahn & Hilliard and the modified Gibbs approach) leadat least for the model system consideredto qualitatively and partly quantitatively equivalent results. Nevertheless, differences remain which may lead to quantitative deviations when applied to the determination of the steady-state nucleation rates and further basic characteristics of nucleation-growth processes. The possible origin of such deviations is discussed, and some further directions of analysis are anticipated

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9.
Инвентарный номер: нет.
   
   B 16


    Baidakov, V. G.
    Boiling-Up Kinetics of Solutions of Cryogenic Liquids / V. G. Baidakov, J. W. P. Schmelzer // Nucleation Theory and Applications. - Berlin : Wiley-VCH Verlag, 2005. - С. 126-175
ББК 53
Рубрики: ФИЗИКА
Кл.слова (ненормированные):
NUCLEATION KINETICS -- DIFFUSION TENSOR OF NUCLEI -- NUCLEATION RATES

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10.
Инвентарный номер: нет.
   
   B 74


    Boltachev, G. Sh.
    Is Gibbs' Thermodynamic Theory of Heterogeneous Systems Really Perfect? / G. Sh. Boltachev, V. G. Baidakov, J. W. P. Schmelzer // Nucleation Theory and Applications. - Berlin : Wiley-VCH Verlag, 2005. - С. 418-446
ББК 53
Рубрики: ФИЗИКА
Кл.слова (ненормированные):
NUCLEATION -- GIBBS' THERMODYNAMIC THEORY -- HETEROGENEOUS SYSTEMS

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