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Effect of Cage Occupancies on Molecular Vibrations of Methane in Structure H Clathrate Hydrate : Ab Initio Molecular Dynamics Simulation
https://tokushima-u.repo.nii.ac.jp/records/2012108
https://tokushima-u.repo.nii.ac.jp/records/2012108ba32b2cf-0c50-4c80-b689-605cfb6c0d22
| 名前 / ファイル | ライセンス | アクション |
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jpcb_128_23_5727.pdf (3.29 MB)
Download is available from 2025/6/4.
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| Item type | 文献 / Documents(1) | |||||||||||||||||||||||
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| 公開日 | 2024-06-18 | |||||||||||||||||||||||
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| アクセス権 | embargoed access | |||||||||||||||||||||||
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| 資源タイプ識別子 | http://purl.org/coar/resource_type/c_6501 | |||||||||||||||||||||||
| 資源タイプ | journal article | |||||||||||||||||||||||
| 出版社版DOI | ||||||||||||||||||||||||
| 関連識別子 | https://doi.org/10.1021/acs.jpcb.4c01790 | |||||||||||||||||||||||
| 関連名称 | 10.1021/acs.jpcb.4c01790 | |||||||||||||||||||||||
| 出版タイプ | ||||||||||||||||||||||||
| 出版タイプ | NA | |||||||||||||||||||||||
| 出版タイプResource | http://purl.org/coar/version/c_be7fb7dd8ff6fe43 | |||||||||||||||||||||||
| タイトル | ||||||||||||||||||||||||
| タイトル | Effect of Cage Occupancies on Molecular Vibrations of Methane in Structure H Clathrate Hydrate : Ab Initio Molecular Dynamics Simulation | |||||||||||||||||||||||
| 著者 |
吉田, 健
× 吉田, 健
WEKO
371
× スハラ, シンノスケ
× 野口, 直樹
WEKO
861
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| 抄録 | ||||||||||||||||||||||||
| 内容記述 | The structure H (sH) of methane hydrate, which has a distinctive structure with large (LL) cages capable of encapsulating multiple methane molecules, has been suggested as a methane reservoir in large icy bodies such as Titan, making it important in planetary science. This high-pressure phase, which exists in the GPa range, lends itself to the study of methane states and dynamics using powerful experimental techniques such as IR and Raman spectroscopy. However, the interpretation of the vibrational spectra of methane in the sH structure has been challenging because of the spectral complexities. The signals attributed to the methane molecules in the LL cage, as well as those of the other two cage types, overlap in the spectra. In this study, we investigated the microscopic origins of the shape of the C–H stretching vibration spectrum of methane in the LL cage using ab initio molecular dynamics (AIMD) simulations. For a single methane molecule in the LL cage, the ν3 band of the C–H stretching mode was observed at a higher frequency typical of isolated molecules in vacuum due to the large size of the LL cage. As the number of methane molecules in the LL cage increased beyond one, a tendency to blue-shift with increasing methane occupancy was observed, consistent with a loose-cage-tight-cage model. By characterizing the time correlation function of methane stretching vibrations based on the solvation number of methane and water molecules proximal to methane within the LL cage, we showed that the complicated spectral line shape observed in cases of higher methane occupancy in the LL cage resulted from the wider variation of the solvation shell states. Analysis of the solvation structures of the AIMD trajectories provided interpretations of the experimental spectral line shape, demonstrating the complementary nature of AIMD to the experiment and its effectiveness in analysis. | |||||||||||||||||||||||
| 書誌情報 |
en : The Journal of Physical Chemistry B 巻 128, 号 23, p. 5727-5734, 発行日 2024-06-04 |
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| 収録物識別子タイプ | ISSN | |||||||||||||||||||||||
| 収録物識別子 | 15206106 | |||||||||||||||||||||||
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| 収録物識別子タイプ | ISSN | |||||||||||||||||||||||
| 収録物識別子 | 15205207 | |||||||||||||||||||||||
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| 収録物識別子タイプ | NCID | |||||||||||||||||||||||
| 収録物識別子 | AA11114073 | |||||||||||||||||||||||
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| 収録物識別子タイプ | NCID | |||||||||||||||||||||||
| 収録物識別子 | AA12189704 | |||||||||||||||||||||||
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| 出版者 | ACS Publications | |||||||||||||||||||||||
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| 権利情報 | This document is the Accepted Manuscript version of a Published Work that appeared in final form in The Journal of Physical Chemistry B, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acs.jpcb.4c01790. | |||||||||||||||||||||||
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| 識別子 | 408626 | |||||||||||||||||||||||
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| 言語 | eng | |||||||||||||||||||||||
