Dielectric relaxation of water: assessing the impact of localized modes, translational diffusion, and collective dynamics

Hölzl, Christoph; Forbert, Harald; Marx, Dominik

doi:10.1039/d1cp03507j

Cited by 19 publications

(11 citation statements)

References 58 publications

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“…Including the electronic polarization and charge transfer effects, the ab initio quantum mechanical calculation has become a progressively more important approach that allows deriving the molecular dipoles through decomposing the electronic structure in terms of maximally localized Wannier orbitals . In a state-of-the-art ab initio and force-field MD simulation work, the dielectric loss spectra in the gigahertz range obtained by the classical force-field still agreed well with that obtained by ab initio MD and dielectric spectroscopy . Thus, the classical force-field is capable of analyzing the γ peak of the spectral response of water as we are interested here.…”

Section: Discussionmentioning

confidence: 61%

“…76 In a state-of-the-art ab initio and force-field MD simulation work, the dielectric loss spectra in the gigahertz range obtained by the classical forcefield still agreed well with that obtained by ab initio MD and dielectric spectroscopy. 77 Thus, the classical force-field is capable of analyzing the γ peak of the spectral response of water as we are interested here. For the higher-frequency domain (around or above 200 GHz), the ab initio MD is more suitable.…”

Section: Introductionmentioning

confidence: 99%

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Stochastic Analysis of Molecular Dynamics Reveals the Rotation Dynamics Distribution of Water around Lysozyme

Matsuura

Shirakashi

2022

J. Phys. Chem. B

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Water dynamics is essential to biochemical processes by mediating all such reactions, including biomolecular degeneration in solutions. To disentangle the molecular-scale distribution of water dynamics around a solute biomolecule, we investigated here the rotational dynamics of water around lysozyme by combining molecular dynamics (MD) simulations and broadband dielectric spectroscopy (BDS). A statistical analysis using the relaxation times and trajectories of every single water molecule was proposed, and the two-dimensional probability distribution of water at a distance from the lysozyme surface with a rotational relaxation time was given. For the observed lysozyme solutions of 34–284 mg/mL, we discovered that the dielectric relaxation time obtained from this distribution agrees well with the measured γ relaxation time, which suggests that rotational self-correlation of water molecules underlies the gigahertz domain of the dielectric spectra. Regardless of protein concentration, water rotational relaxation time versus the distance from the lysozyme surface revealed that the water rotation is severely retarded within 3 Å from the lysozyme surface and is nearly comparable to pure water when farther than 10 Å. The dimension of the first hydration layer was subsequently identified in terms of the relationship between the acceleration of water rotation and the distance from the protein surface.

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Section: Discussionmentioning

confidence: 61%

Section: Introductionmentioning

confidence: 99%

Stochastic Analysis of Molecular Dynamics Reveals the Rotation Dynamics Distribution of Water around Lysozyme

Matsuura

Shirakashi

2022

J. Phys. Chem. B

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“…An inherently powerful spectroscopic tool to study liquid water is terahertz (THz) radiation because it can reveal the fluctuations of the water network on the picosecond time scale. In fact, THz radiation between about 0.01 and 20 THz is strongly absorbed by the intermolecular, collective modes of liquid water [4][5][6][7][8][9][10] .…”

Section: Introductionmentioning

confidence: 99%

Nonlinear TeraHertz Transmission by Liquid Water at 1 THz

Novelli

Adhlakha

et al. 2020

Applied Sciences

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The solvation properties of liquid water originate from the transient network of hydrogen-bonded molecules. In order to probe the coupling between the different modes of this network, nonlinear terahertz (THz) spectroscopy techniques are required. Ideally, these techniques should use a minimal volume and capitalize on sensitive field-resolved detection. Here we performed open aperture z-scan transmission experiments on static liquid cells, and detect the THz fields with electro-optical techniques. We show that it is possible to quantify the nonlinear response of liquid water at ~1 THz even when large signals originate from the sample holder windows.

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“…Thus, our findings vindicate the statement expressed in view of ref. 14 that “Recently, the central role of translational diffusion for dielectric relaxation was explicitly demonstrated by studying isotope effects on the dielectric relaxation spectra.” 63…”

Section: Discussionmentioning

confidence: 99%

Isotope effects on the dynamics of amorphous ices and aqueous phosphoric acid solutions

Ahlmann

Hoffmann

Keppler

et al. 2022

Phys. Chem. Chem. Phys.

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Dielectric relaxation of water: assessing the impact of localized modes, translational diffusion, and collective dynamics

Abstract: A multitude of distinct physical processes and molecular mechanisms have been introduced in the past in an effort to understand the unusual dielectric loss spectrum of water with its pronounced...

Cited by 19 publications

References 58 publications

Stochastic Analysis of Molecular Dynamics Reveals the Rotation Dynamics Distribution of Water around Lysozyme

Stochastic Analysis of Molecular Dynamics Reveals the Rotation Dynamics Distribution of Water around Lysozyme

Nonlinear TeraHertz Transmission by Liquid Water at 1 THz

Isotope effects on the dynamics of amorphous ices and aqueous phosphoric acid solutions

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