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Abstract
The first-order phase transition between two tetrahedral networks of different density—introduced as a hypothesis to account for the anomalous behaviour of certain thermodynamic properties of deeply supercooled water—has received strong support from a growing body of work in recent years. Here we show that this liquid–liquid phase transition in tetrahedral networks can be described as a transition between an unentangled, low-density liquid and an entangled, high-density liquid, the latter containing an ensemble of topologically complex motifs. We first reveal this distinction in a rationally designed colloidal analogue of water. We show that this colloidal water model displays the well-known water thermodynamic anomalies as well as a liquid–liquid critical point. We then investigate water, employing two widely used molecular models, to demonstrate that there is also a clear topological distinction between its two supercooled liquid networks, thereby establishing the generality of this observation, which might have far-reaching implications for understanding liquid–liquid phase transitions in tetrahedral liquids.
Original language | English |
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Pages (from-to) | 1248-1253 |
Number of pages | 6 |
Journal | Nature Physics |
Volume | 18 |
Issue number | 10 |
Early online date | 11 Aug 2022 |
DOIs | |
Publication status | Published - Oct 2022 |
Bibliographical note
Funding Information:We thank M. Dennis, D. Frenkel, F. Leoni, V. N. Manoharan, C. Micheletti and J. Russo for helpful discussions. We also gratefully acknowledge support from the Royal Society via International Exchanges Award IES\R3\183166. A.N. and D.C. thank the Institute of Advanced Studies and the BlueBEAR HPC service of the University of Birmingham. D.C. acknowledges support from the EPSRC Centre for Doctoral Training in Topological Design (EP/S02297X/1). F.S. acknowledges support from Ministero Istruzione Università Ricerca – Progetti di Rilevante Interesse Nazionale (grant 2017Z55KCW) and thanks IscrB-CINECA for providing numerical resources.
Publisher Copyright:
© 2022, The Author(s).
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- 1 Finished
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Polymorph selection in hierarchical self-assembly pathways into open colloidal crystals
1/03/19 → 28/02/22
Project: Research Councils
Datasets
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Research data supporting the publication "Topological Nature of the Liquid-Liquid Phase Transition in Tetrahedral Liquids"
Neophytou, A. (Creator), Chakrabarti, D. (Creator) & Sciortino, F. (Creator), University of Birmingham, 15 Aug 2022
DOI: https://doi.org/10.25500/edata.bham.00000861
Dataset