Critical assessment of the alleged failure of the Classical Nucleation Theory at low temperatures

TL;DR

This study rigorously tests whether the perceived failure of Classical Nucleation Theory at low temperatures is due to non-steady-state data, finding weak evidence for such a breakdown in most datasets.

Contribution

The paper provides a rigorous analysis of nucleation data, demonstrating that the alleged failure of Classical Nucleation Theory at low temperatures is not a universal phenomenon.

Findings

Weak evidence of nucleation break in 2 datasets

Most datasets do not show failure of Classical Nucleation Theory

Steady-state regime validation is crucial for accurate nucleation analysis

Abstract

The Classical Nucleation Theory allegedly fails to describe the temperature dependence of the homogeneous crystal nucleation rates below the temperature of maximum nucleation, $T_{\mathrm{max}}$. Possible explanations for this suspected breakdown have been advanced in the literature. However, the simplest hypothesis has never been tested, that it is a byproduct of nucleation datasets that have not reached the steady-state regime. In this work, we tested this possibility by analyzing published nucleation data for oxide supercooled liquids, using only nucleation and viscosity data measured in samples of the same glass batch that also have satisfied a steady-state regime test. Furthermore, all the uncertainty and regression confidence bands were computed and considered. Having this rigorous protocol, among the 6 datasets analyzed, we only found weak evidence supporting the existence of the nucleation break in 2 datasets. Our collective results thus indicate that the break at $T_{\mathrm{max}}$ is not a common feature of all glass-formers.