Vibrational Response of Hydrogen-Bonded Interfacial Water is Dominated by Intramolecular Coupling

Sovago, Maria; Campen, R. Kramer; Wurpel, George W. H.; Müller, Markus; Bakker, Huib J.; Bonn, Mischa

doi:10.1103/physrevlett.100.173901

Cited by 316 publications

(245 citation statements)

References 27 publications

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“…The fit parameters reflecting the simplification of the SFG spectra upon isotopic dilution are shown in Tables 1 and 2 for the waterlipid and water-protein interfaces, respectively. This observation cannot be reconciled with the presence of two distinct sub-ensembles of strongly ('ice-like') and weakly ('liquid-like') hydrogen-bonded interfacial water [17][18][19][20][21]. If the two peaks are due to two different types of OD groups, i.e.…”

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confidence: 65%

No Ice-Like Water at Aqueous Biological Interfaces

et al. 2012

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The surface vibrational spectrum of water at biological interfaces is often interpreted as having ‘ice-like’ and ‘liquid-like’ components. Here we show that the vibrational spectrum of water at both water–lipid and water–protein interfaces greatly simplifies upon H/D isotopic dilution, which is inconsistent with the presence of ‘ice-like’ structures. The changes in the spectra as a function of isotope content can be explained by intramolecular coupling between bend and stretch vibrations of the water molecules.

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confidence: 65%

No Ice-Like Water at Aqueous Biological Interfaces

et al. 2012

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“…This conclusion has been sharpened for a water surface layer to an interpretation as differently ordered structures termed "ice like" (≈3200 cm −1 ) and "liquid like" (≈3400 cm −1 ) [Shen and Ostroverkhov, 2006]. An alternative interpretation, which is subject to ongoing scientific discussion Shen, 2008, 2009], assigns the whole band to a Fermi resonance resulting from an intramolecular coupling of a stretch vibration with a bending mode overtone vibration of water [Sovago et al, 2008]. Very recently, stimulated by new experimental results of a phase-sensitive VSFG study [Ji et al, 2008], Fan et al [2009] presented yet another interpretation based on molecular dynamics calculations.…”

Section: Oh Spectral Range 321 General Spectral Trendsmentioning

confidence: 99%

Revealing structural properties of the marine nanolayer from vibrational sum frequency generation spectra

Laß¹,

Friedrichs²

2011

J. Geophys. Res.

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Natural nanolayers originating from sea surface and subsurface water samples collected in the Baltic Sea have been investigated using surface‐sensitive vibrational sum frequency generation (VSFG) spectroscopy. Distinct spectral signatures of CH and OH bond stretch vibrations have been detected at wavenumbers ranging from 2700 to 3900 cm−1. Measured water‐air interface spectra as well as observed signal intensity trends are discussed in terms of composition and structure of the natural organic nanolayer. Reasoning was based on the comparison with reference spectra, spectral trends inferred from previous VSFG studies, reported average composition of dissolved organic matter in seawater, and simplified assumption that surfactants can be classified as soluble (wet) and insoluble (dry) surfactants. Wet surfactants have been found to be dominant, and often lipid‐like compounds form a very dense surfactant nanolayer. Supported by comparison spectra of xanthan gum solutions, the observed VSFG spectral signatures were tentatively assigned to lipopolysaccharides or other lipid‐like compounds embedded in colloidal matrices of polymeric material. In addition, VSFG spectra of a polluted harbor water sample and a water sample covered with diesel oil are reported.

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“…The vibrational signatures of an adsorbate in the mid-IR region are sensitive to the local environment, so VSFG spectroscopy can be used in unraveling the adsorbate-adsorbate and adsorbate-substrate interactions. [35][36][37][38][39][40] The input and output beam polarizations of VSFG can be independently controlled to produce information about the molecular orientation of the surface species. 41 The molecular structure and rotational dynamics of CH 3 -Si(111) surfaces has been elucidated using polarization-selected VSFG spectroscopy.…”

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confidence: 99%

Vibrational Sum-Frequency Spectroscopic Investigation of the Structure and Azimuthal Anisotropy of Propynyl-Terminated Si(111) Surfaces

et al. 2017

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Vibrational sum-frequency generation (VSFG) spectroscopy was used to investigate the orientation and azimuthal anisotropy of the C-H stretching modes for propynyl-terminated Si(111) surfaces, Si-C≡C-CH 3 . VSFG spectra revealed symmetric and asymmetric C-H stretching modes in addition to a Fermi resonance mode resulting from the interaction of the asymmetric C-H bending overtone with the symmetric C-H stretching vibration. The polarization dependence of the C-H stretching modes was consistent with the propynyl groups oriented such that the Si-C≡C bond is normal to the Si(111) surface. The azimuthal angle dependence of the resonant C-H stretching amplitude revealed no rotational anisotropy for the symmetric C-H stretching mode and a 3-fold rotational anisotropy for the asymmetric C-H stretching mode in registry with the 3-fold symmetric Si(111) substrate. The results are consistent with expectation that the C-H stretching modes of a -CH 3 group are decoupled from the Si substrate due to a -C≡C-spacer. In contrast, the methyl-terminated Si(111) surface, Si-CH 3 , was previously reported to have pronounced vibronic coupling of the methyl stretch modes to the electronic bath of bulk Si. Vacuum-annealing of propynyl-terminated Si(111) resulted in increased 3-fold azimuthal anisotropy for the symmetric stretch, suggesting that removal of

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Vibrational Response of Hydrogen-Bonded Interfacial Water is Dominated by Intramolecular Coupling

Cited by 316 publications

References 27 publications

No Ice-Like Water at Aqueous Biological Interfaces

No Ice-Like Water at Aqueous Biological Interfaces

Revealing structural properties of the marine nanolayer from vibrational sum frequency generation spectra

Vibrational Sum-Frequency Spectroscopic Investigation of the Structure and Azimuthal Anisotropy of Propynyl-Terminated Si(111) Surfaces

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