DFT Investigations of the Vibrational Spectra and Translational Modes of Ice II

Cao, Jing-Wen; Chen, Jiayi; Qin, Xiao-Ling; Zhu, Xu-Liang; Lu, Ji-Qing; Gu, Yue; Yu, Xu-Hao; Zhang, Peng

doi:10.3390/molecules24173135

Cited by 8 publications

(5 citation statements)

References 30 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…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

Self Cite

View full text Add to dashboard Cite

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.

show abstract

Section: Introductionsupporting

confidence: 57%

Comparative Analysis of Hydrogen-Bonding Vibrations of Ice VI

Wang

Zhu

et al. 2021

ACS Omega

Self Cite

View full text Add to dashboard Cite

show abstract

“…For the dynamic processes, please see the Supporting Information. Later, we also found this phenomenon in ice XIV, XVI, XVII, VIII, VII, II, and XV. − Herein, we explained the two peaks of the most common phase, ice Ih, by comparative analysis with ice XI.…”

Section: Resultsmentioning

confidence: 78%

Origin of Two Distinct Peaks of Ice in the THz Region and Its Application for Natural Gas Hydrate Dissociation

et al. 2019

Self Cite

View full text Add to dashboard Cite

For liquid water in the far-infrared spectrum, phonons of molecular vibrations constitute two bands with a narrow gap at around 30 meV. Interestingly, there are two distinct peaks for ice in this gap. We demonstrated that the two peaks come from two kinds of translational modes. Considering different O–O–O bending constants, we yielded two frequencies based on the ideal model of ice Ic. These two kinds of 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 liquid water. A new method to decompose gas hydrates was proposed by supplying two terahertz radiation energies at ∼6.8 and 9.1 THz. This is also applicable to flow assurance in gas pipelines, aircraft deicers, and so on. Experimental measurements are expected to verify this finding along with the rapid development of a THz laser.

show abstract

“…The INS spectrum showed two distinct Hbond peaks at atmospheric pressure and in some high-pressure ice phases. 21 After a series of investigations, we deduced that these two distinct H-bond peaks were derived from two kinds of H-bond vibrational modes, namely, four-bond and two-bond modes, rather than from two H-bond force constants, as proposed by Li et al [23][24][25][26][27][28]32 In all ice phases, each water molecule is linked to four neighboring water molecules via Hbonds, forming a tetrahedral structure. In the ideal model of hydrogen-ordered ice Ic, the central molecule in the four-bond mode vibrates along the H−O−H angle bisector, while the four neighboring molecules vibrate in the opposite direction.…”

Section: ■ Results and Discussionmentioning

confidence: 93%

“…21 We disagreed with this view 22 and proposed a theory of two intrinsic H-bond vibrational modes. 23 On the basis of a series of studies of ice Ic, 23 II, 24 VII, 25 VIII, 26 X, 27 XV, 28 and others, we deduced that this is a general rule for vibrational modes of the ice family. In this study, we demonstrated how to analyze hydrogen-disordered complex ice V using first-principles density functional theory simulations.…”

Section: ■ Introductionmentioning

confidence: 78%

A Strategy for the Analysis of the Far-Infrared Vibrational Modes of Hydrogen-Disordered Ice V

et al. 2021

Self Cite

View full text Add to dashboard Cite

Analysis of the intermolecular vibrational modes in a fingerprint region is always difficult. It is particularly hard to figure out the normal modes, especially in the far-infrared (IR) region, which represent the collective motion of the lattice skeleton. In this study, we determined a strategy for the analysis of a hydrogen-disordered ice phase, ice V. Its phonon density of states and IR and Raman spectra were calculated and verified by experimental data. The focus of this study was to analyze the hydrogen bond (H-bond) vibrational modes in the terahertz region. We used a density functional theory method to develop analytical formulas to prove the existence of two types of H-bond vibrational modes. In the strong mode, the molecules in the lattice vibrate against four neighbors via H-bond stretching, and in the weak mode, the molecules vibrate along two H-bonds between molecules. The ratio of the vibration energy is approximately √2.

show abstract

DFT Investigations of the Vibrational Spectra and Translational Modes of Ice II

Cited by 8 publications

References 30 publications

Comparative Analysis of Hydrogen-Bonding Vibrations of Ice VI

Comparative Analysis of Hydrogen-Bonding Vibrations of Ice VI

Origin of Two Distinct Peaks of Ice in the THz Region and Its Application for Natural Gas Hydrate Dissociation

A Strategy for the Analysis of the Far-Infrared Vibrational Modes of Hydrogen-Disordered Ice V

Contact Info

Product

Resources

About