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research article

Giant Splitting of the Hydrogen Rotational Eigenenergies in the C2 Filled Ice

Di Cataldo, Simone
•
Rescigno, Maria
•
Monacelli, Lorenzo
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December 6, 2024
Physical Review Letters

Hydrogen hydrates exhibit a rich phase diagram influenced by both pressure and temperature, with the so-called C2 phase emerging prominently above 2.5 GPa. In this phase, hydrogen molecules are densely packed within a cubic icelike lattice and the interaction with the surrounding water molecules profoundly affects their quantum rotational dynamics. Herein, we delve into this intricate interplay by directly solving the Schrödinger's equation for a quantum H2 rotor in the C2 crystal field at finite temperature, generated through density functional theory. Our calculations reveal a giant energy splitting relative to the magnetic quantum number of ±3.2 meV for l=1. Employing inelastic neutron scattering, we experimentally measure the energy levels of H2 within the C2 phase at 6.0 and 3.4 GPa and low temperatures, finding good agreement with our theoretical predictions. These findings underscore the pivotal role of hydrogen-water interactions in dictating the rotational behavior of the hydrogen molecules within the C2 phase and indicate heightened van der Waals interactions compared to other hydrogen hydrates.

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Type
research article
DOI
10.1103/PhysRevLett.133.236101
Scopus ID

2-s2.0-85211465688

PubMed ID

39714703

Author(s)
Di Cataldo, Simone

Sapienza Università di Roma

Rescigno, Maria

Sapienza Università di Roma

Monacelli, Lorenzo

Sapienza Università di Roma

Ranieri, Umbertoluca

The University of Edinburgh

Gaal, Richard  

École Polytechnique Fédérale de Lausanne

Klotz, Stefan

Sorbonne Université

Ollivier, Jacques

Institut Laue-Langevin

Koza, Michael Marek

Institut Laue-Langevin

De Michele, Cristiano

Sapienza Università di Roma

Bove, Livia Eleonora

Sapienza Università di Roma

Date Issued

2024-12-06

Published in
Physical Review Letters
Volume

133

Issue

23

Article Number

236101

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
LQM  
FunderFunding(s)Grant NumberGrant URL

Institut Laue-Langevin

European Union

ANR-23-CE30-0034 EXOTIC-ICE

FNS

212889

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Available on Infoscience
January 25, 2025
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/244462
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