Hydrogen bond symmetrization in high-pressure ice clathrates
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arXiv
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| Autores principales: | , , , , , |
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| Formato: | Preprint |
| Publicado: |
2025
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| _version_ | 1866916795414216704 |
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| author | Monacelli, Lorenzo Rescigno, Maria Nicholls, Alasdair Ranieri, Umbertoluca Di Cataldo, Simone Bove, Livia Eleonora |
| author_facet | Monacelli, Lorenzo Rescigno, Maria Nicholls, Alasdair Ranieri, Umbertoluca Di Cataldo, Simone Bove, Livia Eleonora |
| contents | 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 hydrate (H2-H2O and H2-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 new insight into the quantum-driven mechanisms of bond symmetrization in complex hydrogen-bonded systems under extreme conditions. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2506_13169 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Hydrogen bond symmetrization in high-pressure ice clathrates Monacelli, Lorenzo Rescigno, Maria Nicholls, Alasdair Ranieri, Umbertoluca Di Cataldo, Simone Bove, Livia Eleonora Materials Science 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 hydrate (H2-H2O and H2-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 new insight into the quantum-driven mechanisms of bond symmetrization in complex hydrogen-bonded systems under extreme conditions. |
| title | Hydrogen bond symmetrization in high-pressure ice clathrates |
| topic | Materials Science |
| url | https://arxiv.org/abs/2506.13169 |