Comment on “An interpretation of the low-frequency spectrum of liquid water” [J. Chem. Phys. <b>118</b>, 452 (2003)]

Santis, A. De; Ercoli, Alessandro; Rocca, Dario

doi:10.1063/1.1634251

Cited by 32 publications

(31 citation statements)

References 14 publications

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“…These correspond to the two broad bands centered at about 50 cm −1 and 200 cm −1 , generally addressed in the literature [23][24][25][26] as "bending" and "stretching" modes of the hydrogen-bond network, respectively. At long times the signal shows a monotonic decay; in the first OKE investigations it was interpreted as a bi-exponential relaxation, due to single molecule orientational dynamics 27 .…”

Section: Hd-oke Water Datamentioning

confidence: 99%

Optical Kerr effect of liquid and supercooled water: The experimental and data analysis perspective

Taschin¹,

Bartolini²,

Eramo³

et al. 2014

The Journal of Chemical Physics

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The time-resolved optical Kerr effect spectroscopy (OKE) is a powerful experimental tool enabling accurate investigations of the dynamic phenomena in molecular liquids. We introduced innovative experimental and fitting procedures, that permit a safe deconvolution of sample response function from the instrumental function. This is a critical issue in order to measure the dynamics of sample presenting weak signal, e.g. liquid water. We report OKE data on water measuring intermolecular vibrations and the structural relaxation processes in an extended temperature range, inclusive of the supercooled states. The unpreceded data quality makes possible a solid comparison with few theoretical models; the multi-mode Brownian oscillator model, the Kubo's discrete random jump model and the schematic mode-coupling model. All these models produce reasonable good fits of the OKE data of stable liquid water, i.e. over the freezing point. The features of water dynamics in the OKE data becomes unambiguous only at lower temperatures, i.e. for water in the metastable supercooled phase. Hence this data enable a valid comparison between the model fits. We found that the schematic mode-coupling model provides the more rigorous and complete model for water dynamics, even if is intrinsic hydrodynamic approach hide the molecular informations.

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Section: Hd-oke Water Datamentioning

confidence: 99%

Optical Kerr effect of liquid and supercooled water: The experimental and data analysis perspective

Taschin¹,

Bartolini²,

Eramo³

et al. 2014

The Journal of Chemical Physics

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“…According to the literature [77][78][79][80][81][82][83] , the designation for the low frequency band in the Raman spectrum of liquid water observed experimentally at about 60 cm -1 is still a subject of debate; however it is now accepted that the presence of this band is due to a mixture of underlying mechanisms, including hydrogen bridge bonds and cage effects. The shoulder observed at higher frequencies for the average spectral density…”

Section: E Atomic Translational Dynamics -Spectral Densitiesmentioning

confidence: 99%

Hydrogen Bonding and Related Properties in Liquid Water: A Car–Parrinello Molecular Dynamics Simulation Study

2014

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The local hydrogen bonding structure and dynamics of liquid water have been investigated using the Car-Parrinello molecular dynamics simulation technique. The radial distribution functions and coordination numbers around water molecules have been found to be strongly dependent on the number of hydrogen bonds formed by each molecule, revealing also the existence of local structural heterogeneities in the structure of the liquid. The results obtained have also revealed the strong effect of the local hydrogen bonding network on the local tetrahedral structure and entropy. The investigation of the dynamics of the local hydrogen bonding network in liquid water has shown that this network is very labile and the hydrogen bonds break and reform very rapidly. Nevertheless, it has been found that the hydrogen bonding states associated with the formation of 4 hydrogen bonds by a water molecule exhibit the largest survival probability and corresponding lifetime. The reorientational motions of water molecules have also been found to be strongly dependent on their initial hydrogen bonding state.Finally the dependence of the librational and vibrational modes of water molecules on the local hydrogen bonding network has been carefully examined, revealing a significant effect upon the libration and bond-stretching peak frequencies. The calculated low frequency peaks come in agreement with previously reported interpretations of the experimental low frequency Raman spectrum of liquid water.

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“…A high frequency peak that cannot be observed in the g͑͒ of no associated liquids and has been related to the stretching motions of hydrogen bonded molecules along the bond direction. 16 This interpretation of the microscopic origin of these bands has been partially criticized by De Santis et al, 12 which suggest that the two bands are present in all liquids including no associated liquids. The arguments given by De Santis et al were mainly based on the existence of two bands in the g͑͒ curves for solid Ar at 20 K and quenched amorphous water at 70 K. However, our results show that the high frequency band becomes weakened as temperature increases and is not visible in disordered systems.…”

Section: A Structure and Single Dynamic Propertiesmentioning

confidence: 99%

“…12,16,17 The g͑͒ curves for these systems show two peaks. A low frequency peak that is a characteristic feature of g͑͒ for all sorts of dense liquids and has been attributed to the frustrated translations due to the local structure around a given atom (or molecule) that produces a cage effect.…”

Section: A Structure and Single Dynamic Propertiesmentioning

confidence: 99%

“…The low-frequency peak is mainly associated with the transverse modes whereas the high frequency peak is associated with the longitudinal modes. 11,12 As T increases the peaks become smoothed and the high-frequency peak for C5 appears as a shoulder for C20. In the case of liquids the two peaks cannot be distinguished by observing the shape of the g͑͒ curves but it was shown that the low and high frequency regions of g͑͒ should be also related to the contributions of the transverse and the longitudinal modes, respectively.…”

Section: A Structure and Single Dynamic Propertiesmentioning

confidence: 99%

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Collective dynamic properties in simple crystals: Influence of the structural disorder

Anento¹,

Padró²

2004

Phys. Rev. B

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Collective dynamic properties in Lennard-Jones crystals are investigated by molecular dynamics simulation. The study is focused on properties such as the dynamic structure factors, the longitudinal and transverse currents and the density of states. The influence on these properties of the structural disorder is analyzed by comparing the results for one-component crystals with those for liquids and supercooled liquids at analogous conditions. The effects of species-disorder on the collective properties of binary crystals are also discussed.

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Comment on “An interpretation of the low-frequency spectrum of liquid water” [J. Chem. Phys. 118, 452 (2003)]

Cited by 32 publications

References 14 publications

Optical Kerr effect of liquid and supercooled water: The experimental and data analysis perspective

Optical Kerr effect of liquid and supercooled water: The experimental and data analysis perspective

Hydrogen Bonding and Related Properties in Liquid Water: A Car–Parrinello Molecular Dynamics Simulation Study

Collective dynamic properties in simple crystals: Influence of the structural disorder

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