Crystal melting influenced by particle cooperativity of the liquid

  • Recently, a universal relation between the thermal expansion coefficient of glasses αg, their glass-transition temperature Tg, and the so-called fragility index m of the corresponding supercooled liquid state was found to be valid for more than 200 glass formers, namely αg/m ∝ 1/Tg [Lunkenheimer et al., Nat. Phys. 19, 694 (2023)]. Here we show that this could also have far-reaching consequences for our understanding of crystal melting. Namely, when considering the empirically founded 2/3 rule, stating that the ratio of Tg and the melting temperature Tm is about 2/3 for almost all materials, for crystals a similar relation, αc/m ∝ 1/Tm, should apply. Indeed, we find that the available experimental data are quite consistent with such a relation. This implies that the melting of a crystal into an ordinary (nonsupercooled) liquid is influenced by the fragility, a property quantifying the non-Arrhenius dynamics in the supercooled-liquid state of the material. We argue that this can beRecently, a universal relation between the thermal expansion coefficient of glasses αg, their glass-transition temperature Tg, and the so-called fragility index m of the corresponding supercooled liquid state was found to be valid for more than 200 glass formers, namely αg/m ∝ 1/Tg [Lunkenheimer et al., Nat. Phys. 19, 694 (2023)]. Here we show that this could also have far-reaching consequences for our understanding of crystal melting. Namely, when considering the empirically founded 2/3 rule, stating that the ratio of Tg and the melting temperature Tm is about 2/3 for almost all materials, for crystals a similar relation, αc/m ∝ 1/Tm, should apply. Indeed, we find that the available experimental data are quite consistent with such a relation. This implies that the melting of a crystal into an ordinary (nonsupercooled) liquid is influenced by the fragility, a property quantifying the non-Arrhenius dynamics in the supercooled-liquid state of the material. We argue that this can be explained by a significant enhancement of the “ideal” (noncooperative) melting temperature arising from the cooperativity of the particle motion in the liquid state above Tm. Therefore, a reassessment of the currently widely accepted microscopic understanding of crystal melting, still founded on the general ideas that lead to the time-honored Lindemann melting criterion, may be necessary.show moreshow less

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Metadaten
Author:Peter LunkenheimerORCiDGND, Konrad SamwerORCiD, Alois LoidlORCiDGND
URN:urn:nbn:de:bvb:384-opus4-1159406
Frontdoor URLhttps://opus.bibliothek.uni-augsburg.de/opus4/115940
ISSN:2469-9950OPAC
Parent Title (English):Physical Review B
Publisher:American Physical Society (APS)
Type:Article
Language:English
Year of first Publication:2024
Publishing Institution:Universität Augsburg
Release Date:2024/10/21
Tag:Schmelzen; Wärmeausdehnung; Glasumwandlung; Viskosität
melting; glass transition; viscosity; melting point; thermal expansion
Volume:110
Issue:13
First Page:134110
DOI:https://doi.org/10.1103/PhysRevB.110.134110
Institutes:Mathematisch-Naturwissenschaftlich-Technische Fakultät
Mathematisch-Naturwissenschaftlich-Technische Fakultät / Institut für Physik
Mathematisch-Naturwissenschaftlich-Technische Fakultät / Institut für Physik / Lehrstuhl für Experimentalphysik V
Dewey Decimal Classification:5 Naturwissenschaften und Mathematik / 53 Physik / 530 Physik
Licence (German):Deutsches Urheberrecht