Glasses and the Glass Transition

, by Gutzow, Ivan S.; Mazurin, Oleg V.; Schmelzer, J¿rn W. P.; Todorova, Snejana V.; Petroff, Boris B.; Priven, Alexander I.

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ISBN: 9783527409686 | 3527409688
Cover: Hardcover
Copyright: 5/16/2011

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Written by the best researchers in the field, this up-to-date treatise fills the gap for a high-level work discussing current materials and processes. It covers all the steps involved, from vitrification, relaxation and viscosity, right up to the prediction of glass properties, paving the way for improved methods and applications. For solid state physicists and chemists, materials scientists, and those working in the ceramics industry. With a preface by L. David Pye and a foreword by Edgar D. Zanotto

Foreword	p. V
Preface	p. XVII
Contributors	p. XIX
Introduction	p. 1
Basic Properties and the Nature of Glasses: an Overview	p. 9
Glasses: First Attempts at a Classification	p. 9
Basic Thermodynamics	p. 14
The Fundamental Laws of Classical Thermodynamics and Consequences	p. 14
Thermodynamic Evolution Criteria, Stability Conditions and the Thermodynamic Description of NonequiUbrium States	p. 22
Phases and Phase Transitions: Gibbs's Phase Rule, Ehrenfest's Classification, and the Landau Theory	p. 26
Crystallization, Glass Transition and Devitrification of Glass-Forming Melts: an Overview of Experimental Results	p. 36
The Viscosity of Glass-Jorming Melts	p. 46
Temperature Dependence of the Viscosity	p. 46
Significance of Viscosity in the Glass Transition	p. 54
Molecular Properties Connected with the Viscosity	p. 57
Thermodynamic Properties of Glass-Forming Melts and Glasses: Overview on Experimental Results	p. 59
Heat Capacity	p. 59
Temperature Dependence of the Thermodynamic Functions: Simon's Approximation	p. 65
Further Methods of Determination of Caloric Properties of Glass-Forming Melts and Glasses	p. 74
Change of Mechanical, Optical and Electrical Properties in the Glass Transition Range	p. 76
Thermodynamic Nature of the Glassy State	p. 82
Concluding Remarks	p. 88
Generic Theory of Vitrification of Glass-Forming Melts	p. 91
Introduction	p. 91
Basic Ideas and Equations of the Thermodynamics of Irreversible Processes and Application to Vitrification and Devitrification Processes	p. 95
Basic Assumptions	p. 95
General Thermodynamic Dependencies	p. 96
Application to Vitrification and Devitrification Processes	p. 100
Properties of Glass-Forming Melts: Basic Model Assumptions	p. 103
Kinetics of Relaxation	p. 103
Thermodynamic Properties: Generalized Equation of State	p. 105
Kinetics of Nonisothermal Relaxation as a Model of the Glass Transition: Change of the Thermodynamic Functions in Cyclic Cooling-Heating Processes	p. 207
Description of the Cyclic Processes under Consideration	p. 107
Temperature Dependence of the Structural Order Parameter in Cyclic Cooling and Heating Processes	p. 108
Definition of the Glass Transition Temperature via the Structural Order Parameter: the Bartenev-Ritland Equation	p. 110
Structural Order Parameter and Entropy Production	p. 113
Temperature Dependence of Thermodynamic Potentials at Vitrification	p. 115
Configurational Contributions to Thermodynamic Functions	p. 115
Some Comments on the Value of the Configurational Entropy at Low Temperatures and on the Kauzmann Paradox	p. 112
Cyclic Heating-Cooling Processes: General Results	p. 113
The Prigogine-Defay Ratio	p. 115
Introduction	p. 115
Derivation	p. 117
General Results	p. 117
Quantitative Estimates	p. 133
An Alternative Approach: Jumps of the Thermodynamic Coefficients in Vitrification	p. 135
Comparison with Experimental Data	p. 137
The Prigogine-Defay Ratio	p. 137
Change of Young's Modulus in Vitrification	p. 140
Discussion	p. 142
Fictive (Internal) Pressure and Fictive Temperature as Structural Order Parameters	p. 143
Brief Overview	p. 143
Model-Independent Definition of Fictive (Internal) Pressure and Fictive Temperature	p. 146
On the Behavior of the Viscosity and Relaxation Time at Glass Transition	p. 149
On the Intensity of Thermal Fluctuations in Cooling and Heating of Glass-Forming Systems	p. 152
Introduction	p. 152
Glasses as Systems with Frozen-in Thermodynamic Fluctuations: Mueller and Porai-Koshits	p. 153
Final Remarks	p. 158
Results and Discussion	p. 158
Generic Approach to the Viscosity and the Relaxation Behavior of Glass-Forming Melts	p. 165
Introduction	p. 165
Pressure Dependence of the Viscosity	p. 166
Application of Free Volume Concepts	p. 166
A First Exception: Water	p. 169
Structural Changes of liquids and Their Effect on the Pressure Dependence of the Viscosity	p. 172
Discussion	p. 173
Relaxation Laws and Structural Order Parameter Approach	p. 174
Basic Equations: Aim of the Analysis	p. 174
Analysis	p. 175
Discussion	p. 177
Thermodynamics of Amorphous Solids, Glasses, and Disordered Crystals	p. 179
Introduction	p. 179
Experimental Evidence on Specific Heats and Change of Caloric Properties in Glasses and in Disordered Solids: Simon's Approximations	p. 182
Consequences of Simon's Classical Approximation: the ¿ G(T) Course	p. 194
Change of Kinetic Properties at T_g and the Course of the Vitrification Kinetics	p. 195
The Frenkel-Kobeko Postulate in Terms of the Generic Phenomenological Approach and the Derivation of Kinetic and Thermodynamic Invariants	p. 198
Glass Transitions in Liquid Crystals and Frozen-in Orientational Modes in Crystals	p. 208
Spectroscopic Determination of Zero-Point Entropies in Molecular Disordered Crystals	p. 212
Entropy of Mixing in Disordered Crystals, in Spin Glasses and in Simple Oxide Glasses	p. 213
Generalized Experimental Evidence on the Caloric Properties of Typical Glass-Forming Systems	p. 215
General Conclusions	p. 219
Principles and Methods of Collection of Glass Property Data and Analysis of Data Reliability	p. 223
Introduction	p. 223
Principles of Data Collection and Presentation	p. 225
Main Principles of Data Collection	p. 225
Reasons to Use the Stated Principles of Data Collection	p. 228
Problems in Collecting the Largest Possible Amounts of Glass Property Data	p. 230
Main Principles of Data Presentation	p. 231
Analysis of Existing Data	p. 232
About the Reliability of Experimental Data	p. 232
Analysis of Data on Properties of Binary Systems	p. 233
General Features of the Analysis	p. 233
Some Factors Leading to Gross Errors	p. 237
Some Specific Examples of the Statistical Analysis of Experimental Data	p. 239
What is to Do if the Number of Sources Is Too Small?	p. 243
About the Reliability of the Authors of Publications	p. 246
The Moral Aspect of the Problem	p. 246
An Example of Systematically Unreliable Experimental Data	p. 247
Concluding Remarks	p. 251
General Conclusion	p. 253
Methods of Prediction of Glass Properties from Chemical Compositions	p. 255
Introduction: 120 Years in Search of a Silver Bullet	p. 255
Principle of Additivity of Glass Properties	p. 257
Simple Additive Formulae	p. 257
Additivity and Linearity	p. 258
Deviations from Linearity	p. 259
First Attempts of Simulation of Nonlinear Effects	p. 260
Winkelmann and Schott: Different Partial Coefficients for Different Composition Areas	p. 260
Gehlhoff and Thomas: Simulation of Small Effects	p. 260
Gilard and Dubrul: Polynomial Models	p. 262
Structural and Chemical Approaches	p. 264
Nonlinear Effects and Glass Structure	p. 264
Specifics of the Structural Approach to Glass Property Prediction	p. 266
First Trials of Application of Structural and Chemical Ideas to the Analysis of Glass Property Data	p. 267
Evaluation of the Contribution of Boron Oxide to Glass Properties	p. 267
Model by Huggins and Sun	p. 268
Models by Appen and Demkina	p. 268
Use of Other Structural Characteristics in Appen's and DemMha's Models	p. 271
Recalculation of the Chemical Compositions of Glasses	p. 272
Use of Atomic Characteristics in Glass and Melt Property Prediction Models	p. 278
Ab Initio and Other Direct Methods of Simulation of Glass Structure and Properties	p. 279
Conclusion	p. 280
Simulation of Viscosity of Oxide Glass-Forming Melts in the Twentieth Century	p. 280
Simulation of Viscosity as a Function of Chemical Composition and Temperature	p. 280
Approaches to Simulation of Concentration Dependencies of Viscosity Characteristics	p. 282
Linear Approach	p. 282
Approach of Mazurin: Summarizing of Effects	p. 283
Approach of Lakatos: Redefinition of Variables	p. 284
Polynomial Models	p. 284
Conclusion	p. 285
Simulation of Concentration Dependencies of Glass and Melt Propertie at the Beginning of the Twenty-First Century	p. 286
Global Glass Property Databases as a Catalyst for Development of Glass Property Models	p. 286
Linear and Polynomial Models	p. 286
Calculation of Liquidus Temperature: Neural Network Simulation	p. 28!
Approach of the Author	p. 291
Background	p. 291
Model	p. 292
Comparison with Previous Models	p. 294
Conclusion	p. 296
Fluegel: a Global Model as a Combination of Local Models	p. 296
Integrated Approach: Evaluation of the Most Probable Property Values and Their Errors by Using all Available Models and Large Arrays of Data	p. 297
Simulation of Concentration Dependencies of Glass Properties in Nonoxide Systems	p. 299
Summary: Which Models Were Successful in the Past?	p. 301
Instead of a Conclusion: How to Catch a Bluebird	p. 306
Glasses as Accumulators of Free Energy and Other Unusual Applications of Glasses	p. 311
Introduction	p. 311
Ways to Describe the Glass Transition, the Properties of Glasses and of Defect Crystals: a Recapitulation	p. 313
Simon's Approximation, the Thermodynamic Structural Factor, the Kinetic Fragility of liquids and the Thermodynamic Properties of Defect Crystals	p. 318
The Energy, Accumulated in Glasses and Defect Crystals: Simple Geometric Estimates of Frozen-in Entropy and Enthalpy	p. 324
Enthalpy Accumulated at the Glass Transitions	p. 324
Free Energy Accumulated at the Glass Transition and in Defect Crystals	p. 327
Three Direct Ways to liberate the Energy, Frozen-in in Glasses: Crystallization, Dissolution and Chemical Reactions	p. 332
Solubility of Glasses and Its Significance in Crystal Synthesis and in the Thermodynamics of Vitreous States	p. 332
The Increased Reactivity of Glasses and the Kinetics of Chemical Reactions Involving Vitreous Solids	p. 339
The Fourth Possibility to Release the Energy of Glass: the Glass/Crystal Galvanic Cell	p. 340
Thermoelectric Driving Force at Metallic Glass/Crystal Contacts: the Seebeck and the Peltier Effects	p. 344
Unusual Methods of Formation of Glasses in Nature and Their Technical Significance
Introductory Remarks	p. 348
Agriglasses, Glasses as Nuclear Waste Forms and Possible Medical Applications of Dissolving Organic Glasses	p. 350
Glasses as Amorphous Battery Electrodes, as Battery Electrolytes and as Battery Membranes	p. 352
Photoeffects in Amorphous Solids and the Conductivity of Glasses	p. 353
Some Conclusions and a Discussion of Results and Possibilities	p. 354
Glasses and the Third Law of Thermodynamics	p. 357
Introduction	p. 357
A Brief Historical Recollection	p. 360
The Classical Thermodynamic Approach	p. 363
Nonequilibrium States and Classical Thermodynamic Treatment	p. 366
Zero-Point Entropy of Glasses and Defect Crystals: Calculations and Structural Dependence	p. 368
Thermodynamic and Kinetic Invariants of the Glass Transition	p. 369
Experimental Verification of the Existence of Frozen-in Entropies	p. 371
Principle of Thermodynamic Correspondence and Zero-Point Entropy Calculations	p. 376
A Recapitulation: the Third Principle of Thermodynamics in Nonequilibrium States	p. 377
On the Etymology of the Word "Glass" in European Languages and Some Final Remarks	p. 379
Introductory Remarks	p. 379
"Sirsu", "Shvistras", "Hyalos","Vitrum", "Glaes", "Staklo", "Cam"	p. 380
"Vitreous", "Glassy" and "Glasartig", "Vitro-crystalline"	p. 382
Glasses in Byzantium, in Western Europe, in Venice, in the Balkans and Several Other Issues	p. 384
Concluding Remarks	p. 385
References	p. 387
Index	p. 407
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Glasses and the Glass Transition

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