Vibrational Spectra of Deuterated Methane and Water Molecules in Structure I Clathrate Hydrate from ab initio MD simulation
Vibrational Spectra of Deuterated Methane and Water Molecules in Structure I Clathrate Hydrate from ab initio MD simulation
复制标题
从头开始 MD 模拟得到的结构 I 笼形水合物中氘代甲烷和水分子的振动光谱
DOI：
10.1080/08927022.2014.929125
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发表时间：
2015
影响因子：
2.1
通讯作者：
and Kenji Yasuoka
中科院分区：
文献类型：
--
作者：
Masaki Hiratsuka;Ryo Ohmura;Amadeu K. Sum;and Kenji Yasuoka
笼形水合物中晶格分子的氘化是一种广泛使用的实验技术，可以清楚地分离振动模式。然而，氘化对振动光谱和分子运动的影响还没有完全了解。由于主客体耦合作用可能改变氘代笼形水合物的振动光谱，因此详细分析氘代笼形水合物的振动光谱对于理解其振动位移的机理具有重要意义。本文采用从头算分子动力学方法计算了氘代甲烷水合物的振动光谱。计算了D_2O晶格中甲烷和H_2O晶格中氘代甲烷的分子内振动频率，并与纯甲烷水合物进行了比较。还报道了弯曲模态的弯曲、摇摆和泛音。揭示了客体分子和主体分子的振动耦合对振动光谱的影响。
The deuteration of the lattice molecules in clathrate hydrates is a widely used experimental technique to clearly separate the vibrational modes. However, the effect of the deuteration on the vibrational spectra and molecular motions is not fully understood. Since the guest–host coupling may change the vibrational spectra, a detailed analysis of the vibrational spectra of deuterated clathrate hydrate is significant in the understanding of the mechanism of the vibrational shift. In this study, the vibrational spectra of the deuterated methane hydrates were calculated byab initiomolecular dynamics simulation. The intramolecular vibrational frequency of the methane in D2O lattice and deuterated methane in H2O lattice was calculated and compared with the pure methane hydrate. The bending, rocking and overtone of the bending mode was also reported. The effect of coupling of the rattling motions of guest and host molecules on the vibrational spectra was revealed.