Reply to "Comment on 'Glass Transition, Crystallization of Glass-Forming Melts, and Entropy"' by Zanotto and Mauro.

Jürn W P Schmelzer,Timur V Tropin

doi:10.3390/e20090704

Abstract

A response is given to a comment of Zanotto and Mauro on our paper published in Entropy 20, 103 (2018). Our arguments presented in this paper are widely ignored by them, and no new considerations are outlined in the comment, which would require a revision of our conclusions. For this reason, we restrict ourselves here to a brief response, supplementing it by some additional arguments in favor of our point of view not included in our above-cited paper.

Highlights

The main part of our paper [1] and the comment on it [2] are concerned with the questions: (i) whether continuous relaxation has to be included in the definition of glass; (ii) whether glasses always crystallize;, (iii) how kinetic criteria of glass transition can be formulated most appropriately; and (iv) whether glasses have a residual entropy or not
(ii) we demonstrated that it is not the relation between experimental observation time, not specified by Zanotto and Mauro in [3], and structural relaxation time that leads to a glass formation in cooling or similar processes, but the interplay between the characteristic time of change of external control parameters and relaxation time
In [1], we already discussed the paper by Goldstein [41] showing that a zero value of the residual entropy violates the second law of thermodynamics

Summary

Introduction

The main part of our paper [1] and the comment on it [2] are concerned with the questions:. (i) whether continuous relaxation has to be included in the definition of glass; (ii) whether glasses always crystallize; (as suggested by Zanotto and Mauro in [3]), (iii) how kinetic criteria of glass transition can be formulated most appropriately; and (iv) whether glasses have a residual entropy or not. The differences between our and Zanotto and Mauro’s points of view were described comprehensively in our paper [1]. We provide here a brief response and supplement it by additional arguments not included in [1]

Definition of Glass and the Glass Transition

Greek Philosophy and Kinetic Criteria of Glass Formation

Temperature Dependence of the Viscosity

Crystallization

Broken Ergodicity and Entropy

Final Remarks