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| Main Authors: | , , , , , |
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| Format: | Preprint |
| Published: |
2025
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| Subjects: | |
| Online Access: | https://arxiv.org/abs/2512.16819 |
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| _version_ | 1866912774182928384 |
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| author | Martin-Gondre, L. Fotso, V. Meko Métais, C. Patt, A. Ollivier, J. Desmedt, A. |
| author_facet | Martin-Gondre, L. Fotso, V. Meko Métais, C. Patt, A. Ollivier, J. Desmedt, A. |
| contents | Thermodynamic stability of N$_2$ clathrate hydrates in the sI and sII structures is investigated using density functional theory with several exchange-correlation functionals, explicitly accounting for composition (cage occupancies) and pressure at T = 0 K. Among the tested functionals, revPBE-D3(0) best reproduces experimental lattice parameters and bulk moduli B$_0$ . Energetic analyses confirm the strong impact of large cage double occupancy on sI, whereas the convex-hull results show that sI with single occupancy remains thermodynamically stable up to $\sim$ 0.8 GPa alongside sII with single occupancy. Increasing pressure then stabilizes sII with double occupancy, consistent with its larger large-cage volume and lower framework strain. These results provide a coherent, first-principles thermodynamic framework for N$_2$ hydrate stability and a baseline for finite-temperature extension. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2512_16819 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Thermodynamical study of N$_2$ clathrate hydrate from DFT calculations Martin-Gondre, L. Fotso, V. Meko Métais, C. Patt, A. Ollivier, J. Desmedt, A. Materials Science Computational Physics Thermodynamic stability of N$_2$ clathrate hydrates in the sI and sII structures is investigated using density functional theory with several exchange-correlation functionals, explicitly accounting for composition (cage occupancies) and pressure at T = 0 K. Among the tested functionals, revPBE-D3(0) best reproduces experimental lattice parameters and bulk moduli B$_0$ . Energetic analyses confirm the strong impact of large cage double occupancy on sI, whereas the convex-hull results show that sI with single occupancy remains thermodynamically stable up to $\sim$ 0.8 GPa alongside sII with single occupancy. Increasing pressure then stabilizes sII with double occupancy, consistent with its larger large-cage volume and lower framework strain. These results provide a coherent, first-principles thermodynamic framework for N$_2$ hydrate stability and a baseline for finite-temperature extension. |
| title | Thermodynamical study of N$_2$ clathrate hydrate from DFT calculations |
| topic | Materials Science Computational Physics |
| url | https://arxiv.org/abs/2512.16819 |