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research article

Hydrogen bond symmetrization in high-pressure ice clathrates

Monacelli, Lorenzo
•
Rescigno, Maria
•
Nicholls, Alasdair  
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December 8, 2025
Physical Review B

Hydrogen bond symmetrization is a fundamental pressure-induced transformation in which the distinction between donor and acceptor sites vanishes, resulting in a symmetric hydrogen-bond network. While extensively studied in pure ice—most notably during the ice VII to ice X transition—this phenomenon remains less well characterized in hydrogen hydrates. In this work, we investigate hydrogen bond symmetrization in the high-pressure phases of hydrogen hydrates (H2-H2OandD2-D2O) through a combined approach of Raman spectroscopy and first-principles quantum atomistic simulations. We focus on the C2 and C3 filled-ice phases, using both hydrogenated and deuterated water frameworks. Our results reveal that quantum fluctuations and the interaction between the encaged H2 molecules and the host lattice play a crucial role in driving the symmetrization process. Remarkably, we find that in both C2 and C3 phases hydrogen bond symmetrization occurs via a continuous crossover at significantly lower pressures than in pure ice, without any change in the overall crystal symmetry. These findings provide insight into the quantum-driven mechanisms of bond symmetrization in complex hydrogen-bonded systems under extreme conditions.

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Type
research article
DOI
10.1103/1cgl-mklx
Scopus ID

2-s2.0-105025713832

Author(s)
Monacelli, Lorenzo

Sapienza Università di Roma

Rescigno, Maria

Sapienza Università di Roma

Nicholls, Alasdair  

École Polytechnique Fédérale de Lausanne

Ranieri, Umbertoluca

The University of Edinburgh

Di Cataldo, Simone

Sapienza Università di Roma

Bove, Livia Eleonora  

École Polytechnique Fédérale de Lausanne

Date Issued

2025-12-08

Published in
Physical Review B
Volume

112

Issue

21

Start page

1

End page

8

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
LQM  
Available on Infoscience
January 5, 2026
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/257488
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