The intermolecular dynamics of liquid water

Castner, Edward W.; Chang, Yu Ping; Chu, Y. C.; Walrafen, G. E.

doi:10.1063/1.469177

Cited by 252 publications

(234 citation statements)

References 30 publications

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“…The mode is similar to a mode observed in liquid D 2 O at 170-180 cm −1 . 46,47 In our case the frequency is somewhat lower, as should be expected from the mass difference between NMA and D 2 O. The presence of a resonance close to the energy gap between amide-I and amide-II modes in our simulation lends further support to the suggestion by Wang and Hochstrasser 48 that solvent modes play an important role in the relaxation process.…”

Section: A Fluctuationssupporting

confidence: 75%

Vibrational relaxation in simulated two-dimensional infrared spectra of two amide modes in solution

Dijkstra¹,

Jansen²,

Bloem³

et al. 2007

The Journal of Chemical Physics

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Two-dimensional infrared spectroscopy is capable of following the transfer of vibrational energy between modes in real time. We develop a method to include vibrational relaxation in simulations of two-dimensional infrared spectra at finite temperature. The method takes into account the correlated fluctuations that occur in the frequencies of the vibrational states and in the coupling between them as a result of interaction with the environment. The fluctuations influence the two-dimensional infrared line shape and cause vibrational relaxation during the waiting time, which is included using second-order perturbation theory. The method is demonstrated by applying it to the amide-I and amide-II modes in N-methylacetamide in heavy water. Stochastic information on the fluctuations is obtained from a molecular dynamics trajectory, which is converted to time dependent frequencies and couplings with a map from a density functional calculation. Solvent dynamics with the same frequency as the energy gap between the two amide modes lead to efficient relaxation between amide-I and amide-II on a 560fs time scale. We show that the cross peak intensity in the two-dimensional infrared spectrum provides a good measure for the vibrational relaxation.

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Section: A Fluctuationssupporting

confidence: 75%

Vibrational relaxation in simulated two-dimensional infrared spectra of two amide modes in solution

Dijkstra¹,

Jansen²,

Bloem³

et al. 2007

The Journal of Chemical Physics

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“…proteins, 7,13,14 and carbohydrates 15 have been the subject of a 44 large number of studies in recent years. It is established that the 45 dynamics of hydration water are distinct from those of bulk 46 water; 16 however, the nature and extent of these differences are 47 still a matter of debate.…”

Section: à12mentioning

confidence: 99%

Water Dynamics at Protein Interfaces: Ultrafast Optical Kerr Effect Study

2011

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water. The most marked slowdown was observed for the most hydrophilic protein studied, bovine serum albumin, whereas the most 17 hydrophobic protein, trypsin, had a slightly smaller effect. The terahertz Raman spectra of these protein solutions resemble those of 18 pure water up to a concentration of 5 wt %, above which a new feature appears at ∼80 cm À1 , which is assigned to a bending of the 19 protein amide chain.

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“…7 shows the OKE spectrum of liquid water at room temperature where the translational diffusional (cage-rattling) mode is accompanied by two modes: the hydrogen-bond bend and stretch or, equivalently, the transverse acoustic (TA) and longitudinal acoustic (LA) phonon modes. [35,[111][112][113][114] For water, with its relatively stiff bonding, these are readily identified. In Fig.…”

Section: Universal Behavior?mentioning

confidence: 99%

Rattling the cage: Micro- to mesoscopic structure in liquids as simple as argon and as complicated as water

Turton

Hunger

Stoppa

et al. 2011

Journal of Molecular Liquids

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ÔØ Å ÒÙ× Ö ÔØThis is a PDF file of an unedited manuscript that has been accepted for publication. As a service to our customers we are providing this early version of the manuscript. The manuscript will undergo copyediting, typesetting, and review of the resulting proof before it is published in its final form. Please note that during the production process errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal pertain. Abstract. The water molecule has the convenient property that its molecular polarizability tensor is nearly isotropic while its dipole moment is large. As a result, the low-frequency anisotropic Raman spectrum of liquid water is mostly collision induced and therefore reports primarily translational motions while the far-infrared (terahertz) and dielectric spectrum is dominated by rotational modes. A C C E P T E D M A N U S C R I P T ACCEPTED MANUSCRIPTAtomic and globular-molecular liquids have a zero dipole moment as well as an isotropic polarizability tensor. These spectrum-simplifying properties were exploited in a study of a number of liquids and solutions using ultrafast optical Kerr-effect (OKE) spectroscopy combined with dielectric relaxation spectroscopy (DRS), terahertz time-domain spectroscopy (THz-TDS), and terahertz field-induced second-harmonic generation (TFISH) spectroscopy. For room-temperature ionic liquids (RTILs), liquid water, aqueous salt solutions, noble gas liquids, and globular molecular liquids it was found that, in each case, surprising structure and/or inhomogeneity is observed, ranging from mesoscopic clustering in RTILs to stretched exponential dynamics in the noble gas liquids. For aqueous electrolyte solutions it is shown that the viscosity, normally described by the Jones-Dole expression, can be explained in terms of a jamming transition, a concept borrowed from soft condensed matter studies of glass transitions in colloidal suspensions.

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The intermolecular dynamics of liquid water

Cited by 252 publications

References 30 publications

Vibrational relaxation in simulated two-dimensional infrared spectra of two amide modes in solution

Vibrational relaxation in simulated two-dimensional infrared spectra of two amide modes in solution

Water Dynamics at Protein Interfaces: Ultrafast Optical Kerr Effect Study

Rattling the cage: Micro- to mesoscopic structure in liquids as simple as argon and as complicated as water

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