Jedlovszky, Pal;
Dellago, Christoph;
Sega, Marcello;
(2025)
Hydrogen bond topology reveals layering of LDL-like and HDL-like water at its liquid/vapor interface.
The Journal of Chemical Physics
, 163
(2)
, Article 024511. 10.1063/5.0272802.
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Abstract
The discovery of high-density liquid (HDL) and low-density liquid (LDL) water has been a major success of molecular simulations, yet extending this analysis to interfacial water is challenging due to conventional order parameters assuming local homogeneity. This limitation previously prevented resolving the composition of the surface layer of the liquid/vapor interface. Here, we apply a recently introduced topological order parameter [R. Foffi and F. Sciortino, J. Phys. Chem. B 127, 378-386 (2022)] to analyze the composition of the water/vapor interface across a broad temperature range. Our results reveal that LDL-like water dominates the outermost region at all temperatures, while HDL-like water accumulates beneath it, presenting a clear layering roughly below the temperature of maximum density. This structured stratification, previously inaccessible, highlights the power of the topological order parameter in resolving interfacial molecular heterogeneity and provides new insights into the structural properties of water at interfaces.
| Type: | Article |
|---|---|
| Title: | Hydrogen bond topology reveals layering of LDL-like and HDL-like water at its liquid/vapor interface |
| Location: | United States |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1063/5.0272802 |
| Publisher version: | https://doi.org/10.1063/5.0272802 |
| Language: | English |
| Additional information: | © 2025 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution (CC BY) license (https://creativecommons.org/licenses/by/4.0/). https://doi.org/10.1063/5.0272802 |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10211213 |
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