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research article

Observation of the most H2-dense filled ice under high pressure

Ranieri, Umbertoluca
•
Di Cataldo, Simone
•
Rescigno, Maria  
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December 26, 2023
Proceedings Of The National Academy Of Sciences Of The United States Of America (PNAS)

Hydrogen hydrates are among the basic constituents of our solar system's outer planets, some of their moons, as well Neptune-like exo-planets. The details of their high-pressure phases and their thermodynamic conditions of formation and stability are fundamental information for establishing the presence of hydrogen hydrates in the interior of those celestial bodies, for example, against the presence of the pure components (water ice and molecular hydrogen). Here, we report a synthesis path and experimental observation, by X-ray diffraction and Raman spectroscopy measurements, of the most H2-dense phase of hydrogen hydrate so far reported, namely the compound 3 (or C3). The detailed characterisation of this hydrogen-filled ice, based on the crystal structure of cubic ice I (ice Ic), is performed by comparing the experimental observations with first-principles calculations based on density functional theory and the stochastic self-consistent harmonic approximation. We observe that the extreme (up to 90 GPa and likely beyond) pressure stability of this hydrate phase is due to the close-packed geometry of the hydrogen molecules caged in the ice Ic skeleton.

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Type
research article
DOI
10.1073/pnas.2312665120
Web of Science ID

WOS:001146713500002

Author(s)
Ranieri, Umbertoluca
Di Cataldo, Simone
Rescigno, Maria  
Monacelli, Lorenzo  
Gaal, Richard  
Santoro, Mario
Andriambariarijaona, Leon
Parisiades, Paraskevas
De Michele, Cristiano
Bove, Livia Eleonora  
Date Issued

2023-12-26

Publisher

National Academy of Sciences

Published in
Proceedings Of The National Academy Of Sciences Of The United States Of America (PNAS)
Volume

120

Issue

52

Article Number

e2312665120

Subjects

Clathrate Hydrates

•

Phase Transitions

•

Pressure

•

Raman

•

Ab

•

Initio Simulations

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
LQM  
FunderGrant Number

Swiss National Fund (FNS) grant EXOTIC-ICES

212889

CINECA

RM120172B8E7BC07

Vienna Scientific Cluster

IsC90-HTS-TECH

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Available on Infoscience
February 23, 2024
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/205324
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