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Updated: Jun 19, 2026

Computation of Atmospheric Concentrations of Molecular Clusters from ab initio Thermochemistry
Published on: April 8, 2020
Raman spectroscopy and cage occupancy of hydrogen clathrate hydrate from first-principle calculations
Jianwei Wang1, Hailong Lu, John A Ripmeester
1Department of Geological Sciences, University of Michigan, Ann Arbor, Michigan 48109, USA. jwwang@umich.edu
Abstract:
Statistically averaged Raman spectra of H(2) in hydrogen clathrate are calculated by quantum-mechanical calculations and molecular dynamics simulations. The result shows that the H(2) molecules in the large cages and singly occupied small cages are loosely encaged and the vibrational modes are softened and uncoupled, while those in the doubly occupied small cages are tightly confined, the vibrational modes are strongly coupled, and the frequencies are blue-shifted relative to the free gas. This finding provides important new insights on characterizing the cage occupancy and could inspire innovative experiments for synthesizing the clathrate as a hydrogen storage medium.
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