Computing Investigations of Molecular and Atomic Vibrations of Ice IX

Zhao, Zeng-Ji; Qin, Xiao-Ling; Cao, Jing-Wen; Zhu, Xu-Liang; Yang, Ye-Chen; Wang, Haocheng; Zhang, Peng

doi:10.1021/acsomega.9b03190

Cited by 4 publications

(5 citation statements)

References 36 publications

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“…We have reviewed the vibrational normal modes of ice XV and clarified the physical aspects of its exotic vibrational modes . The distributions of vibrational modes in ice XV are similar to those we have determined in our previous series of studies, such as ice VII and VIII, and the hydrogen-bonding modes in the translational band also obey the theory of two types of hydrogen bonds. − Based on a successful investigation of ice XV, in this study, we constructed an ice VI supercell, explored its atomic and molecular vibrational modes, and compared these modes with those of ice XV. A comparative analysis was also reported in the meaning of an experimental method.…”

Section: Introductionsupporting

confidence: 57%

Comparative Analysis of Hydrogen-Bonding Vibrations of Ice VI

Wang

Zhu

et al. 2021

ACS Omega

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It is difficult to investigate the hydrogen-bonding dynamics of hydrogen-disordered ice VI. Here, we present a comparative method based on our previous study of its counterpart hydrogen-ordered phase, ice XV. The primitive cell of ice XV is a 10 molecule unit, and the vibrational normal modes were analyzed individually. We constructed an 80 molecule supercell of ice VI to mimic the periodic unit and performed first-principles density functional theory calculations. As the two vibrational spectra show almost identical features, we compared the molecular translation vibrations. Inspired by the phonon analysis of ice XV, we found that the vibrational modes in the translation band of ice VI are classifiable into three groups. The lowest-strength vibration modes represent vibrations between two sublattices that lack hydrogen bonding. The highest-strength vibration modes represent the vibration of four hydrogen bonds of one molecule. The middle-strength vibration modes mainly represent the molecular vibrations of only two hydrogen bonds. Although there are many overlapping stronger and middle modes, there are only two main peaks in the inelastic neutron scattering (INS) spectra. This work explains the origin of the two main peaks in the far-infrared region of ice VI and illustrates how to analyze a hydrogen-disordered ice structure.

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Section: Introductionsupporting

confidence: 57%

Comparative Analysis of Hydrogen-Bonding Vibrations of Ice VI

Wang

Zhu

et al. 2021

ACS Omega

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“…一般而言, 随着压强的增加, 氢键键长变短, 氢键强度应增强. 但冰VIII和冰XV [142] 是个特殊的例子. 这归因于它们特殊的结构, 冰 VIII和冰XV皆是由两个子晶格相互套构而成的, (单位: cm -1 ), 结构优化密度(单位: g/cm -3 ) Table 2.…”

Section: 冰Ic理想模型中的两类本征振动unclassified

Investigation of hydrogen bond vibrations of ice

Qin¹,

Zhu²,

Cao³

et al. 2021

Acta Phys. Sin.

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Despite its simple molecular structure, water is still a mystery to scientists. For the atomic and molecular vibrational modes of ice, as is well known, there are two kinds of vibrations: intra-molecular O—H stretching vibration and H—O—H bending vibration within the molecules and three kinds of molecular spatial rotations. However, thirty years ago, a high flux inelastic neutron scattering experiment showed that there are two distinct characteristic peaks in the far-infrared molecular translational vibration region of many ice phases. The origins of these peaks have not been determined till now. In this work, based on the CASTEP code, a first-principles density functional theory plane wave programme, the vibrational spectra as well as the vibrational normal modes of a series of ice phases are investigated. Two kinds of intrinsic hydrogen bond vibrational modes are first found in hydrogen-ordered ice Ic. Then it is found to be a general rule among ice family. Based on the ideal model, we prove that the two vibrational modes can be classified as four-bond vibration and two-bond vibration. There are many coupling modes in-between due to tetrahedral structure deformation under high pressure. Besides, there are also some optical vibrational modes with lower energy in the translational region, such as cluster vibrations and inter-plane vibrations. In Ice VII/VIII and XV/VI, each of which consists of two sublattices, there exist non-hydrogen bond vibrations. These molecular translational vibrations can explain all the far-infrared vibrational spectrum of ice phase, which makes up the last piece of the jigsaw puzzle for the molecular vibration theory of ice. The two vibrational modes do not exist in liquid water due to the collapse of the rigid tetrahedral structure. Thus, a window remains for ice resonance absorption with minimum energy loss in water. This theory is expected to be applicable to industrial deicing, food thawing, gas hydrate mining, and biomolecule frozen molding, etc.

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“…The PDOS of ices III and IX are consistent with their respective INS spectra. In the translation band, it is clear that the two typical HB peaks are at approximately 200 cm −1 and 300 cm −1 for ice IX [20], whereas there is a flat vibrational band for ice III in the same region. To analyze the HBs of ice III, we first introduce the theory of two kinds of intrinsic HB vibrational modes in ice.…”

Section: Resultsmentioning

confidence: 98%

“…Two kinds of intrinsic HB vibrational modes, denoted two-bond and four-bond modes, were found for the ideal ice Ic [21]. A series of investigations of the ice phases has revealed that this is a general rule for the ice family and may successfully explain their far-IR band [18][19][20]. In the present study, we theoretically analyzed the vibrational modes in the translation band to identify the characteristic HB vibrations of ice III in comparison with those of the H-ordered ice IX.…”

Section: Introductionmentioning

confidence: 95%

“…Since two distinct peaks in the far-infrared (IR) region of ice were first probed in the 1990s by inelastic neutron scattering (INS) experiments [15][16][17], the origin of these two vibrational peaks has remained a controversial issue [18][19][20]. Using first-principles density functional theory (DFT), we developed an approach to determine the lattice dynamic process of the crystal vibrational spectrum.…”

Section: Introductionmentioning

confidence: 99%

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Computational Analysis of Hydrogen Bond Vibrations of Ice III in the Far-Infrared Band

et al. 2022

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The hydrogen-disordered structure of ice III makes it difficult to analyze its vibrational spectrum theoretically. To clarify the contribution of hydrogen bonds (HBs), we constructed a 24-molecule supercell to mimic the real structure and performed first-principles density functional theory calculations. The calculated curve of phonon density of states showed good correspondence with the experimental data. Based on the theory of two kinds of HB vibrational modes, we analyzed the distributions of two-bond modes and four-bond modes. The energy splitting of these modes results in a flat vibrational band, which is a common phenomenon in high-pressure ice phases. These findings verified the general rule that there are two types of HB vibrations in ice, thereby furthering our understanding of HB interactions in water ice and their broad role in nature.

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Computing Investigations of Molecular and Atomic Vibrations of Ice IX

Cited by 4 publications

References 36 publications

Comparative Analysis of Hydrogen-Bonding Vibrations of Ice VI

Comparative Analysis of Hydrogen-Bonding Vibrations of Ice VI

Investigation of hydrogen bond vibrations of ice

Computational Analysis of Hydrogen Bond Vibrations of Ice III in the Far-Infrared Band

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