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

Padró, J. A.; Martı́, Jordi

doi:10.1063/1.1634252

Cited by 53 publications

(53 citation statements)

References 15 publications

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“…The first peak is usually related to hindered vibrations of a water molecule in the cage of its nearest neighbors (rattling in a cage), whereas the band centered around 200 cm −1 is associated with stretching vibrations of hydrogen-bonds. 63 The disappearance of this second peak seems to suggest that water molecules in contact with lipid sites tend to form a lower number of hydrogen-bonds.…”

Section: E Spectral Densities Of Water and Lipid Speciesmentioning

confidence: 99%

Diffusion and spectroscopy of water and lipids in fully hydrated dimyristoylphosphatidylcholine bilayer membranes

Yang

Calero

Martı́

2014

The Journal of Chemical Physics

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Microscopic structure and dynamics of water and lipids in a fully hydrated dimyristoylphosphatidylcholine phospholipid lipid bilayer membrane in the liquid-crystalline phase have been analyzed with all-atom molecular dynamics simulations based on the recently parameterized CHARMM36 force field. The diffusive dynamics of the membrane lipids and of its hydration water, their reorientational motions as well as their corresponding spectral densities, related to the absorption of radiation, have been considered for the first time using the present force field. In addition, structural properties such as density and pressure profiles, a deuterium-order parameter, surface tension, and the extent of water penetration in the membrane have been analyzed. Molecular self-diffusion, reorientational motions, and spectral densities of atomic species reveal a variety of time scales playing a role in membrane dynamics. The mechanisms of lipid motion strongly depend on the time scale considered, from fast ballistic translation at the scale of picoseconds (effective diffusion coefficients of the order of 10 −5 cm 2 /s) to diffusive flow of a few lipids forming nanodomains at the scale of hundreds of nanoseconds (diffusion coefficients of the order of 10 −8 cm 2 /s). In the intermediate regime of subdiffusion, collisions with nearest neighbors prevent the lipids to achieve full diffusion. Lipid reorientations along selected directions agree well with reported nuclear magnetic resonance data and indicate two different time scales, one about 1 ns and a second one in the range of 2-8 ns. We associated the two time scales of reorientational motions with angular distributions of selected vectors. Calculated spectral densities corresponding to lipid and water reveal an overall good qualitative agreement with Fourier transform infrared spectroscopy experiments. Our simulations indicate a blue-shift of the low frequency spectral bands of hydration water as a result of its interaction with lipids. We have thoroughly analyzed the physical meaning of all spectral features from lipid atomic sites and correlated them with experimental data. Our findings include a "wagging of the tails" frequency around 30 cm −1 , which essentially corresponds to motions of the tail-group along the instantaneous plane formed by the two lipid tails, i.e., in-plane oscillations are clearly of bigger importance than those along the normal-to-the plane direction. © 2014 AIP Publishing LLC.

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Section: E Spectral Densities Of Water and Lipid Speciesmentioning

confidence: 99%

Diffusion and spectroscopy of water and lipids in fully hydrated dimyristoylphosphatidylcholine bilayer membranes

Yang

Calero

Martı́

2014

The Journal of Chemical Physics

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“…The influence of sugars on the dynamics of water was first probed with the low-frequency VDOS of water, shown for the different trehalose solutions at 293 K in Fig and has also been observed both in hydrogen-bonded and nonassociated liquids [35,36]. It broadens with the addition of sugars, which may reflect the increased heterogeneity of the local environments sampled by water molecules in mixed solutions.…”

Section: Low-frequency Vibrational Dynamicsmentioning

confidence: 99%

Slowing down of water dynamics in disaccharide aqueous solutions

Lerbret¹,

Affouard²,

Bordat³

et al. 2011

Journal of Non-Crystalline Solids

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The dynamics of water in aqueous solutions of three homologous disaccharides, namely trehalose, maltose and sucrose, has been analyzed by means of molecular dynamics simulations in the 0-66 wt % concentration range. The low-frequency vibrational densities of states (VDOS) of water were compared with the susceptibilities chi" of 0-40 wt % solutions of trehalose in D2O obtained from complementary Raman scattering experiments. Both reveal that sugars significantly stiffen the local environments experienced by water. Accordingly, its translational diffusion coefficient decreases when the sugar concentration increases, as a result of an increase of water-water hydrogen bonds lifetimes and of the corresponding activation energies. This induced slowing down of water dynamics, ascribed to the numerous hydrogen bonds that sugars form with water, is strongly amplified at concentrations above 40 wt % by the percolation of the hydrogen bond network of sugars, and may partially explain their well-known stabilizing effect on proteins in aqueous solutions.Comment: 14 pages, 4 figures, accepted in Journal of Non-Crystalline Solids (proceedings of the conference IDMRCS6

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

Abstract: On the accuracy of the MB-pol many-body potential for water: Interaction energies, vibrational frequencies, and classical thermodynamic and dynamical properties from clusters to liquid water and ice

Cited by 53 publications

References 15 publications

Diffusion and spectroscopy of water and lipids in fully hydrated dimyristoylphosphatidylcholine bilayer membranes

Diffusion and spectroscopy of water and lipids in fully hydrated dimyristoylphosphatidylcholine bilayer membranes

Slowing down of water dynamics in disaccharide aqueous solutions

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

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