Communication: Vibrational sum-frequency spectrum of the air-water interface, revisited

Ni, Yicun; Skinner, James

doi:10.1063/1.4958967

Cited by 70 publications

(85 citation statements)

References 29 publications

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“…Proper treatment of absorptive-dispersive interactions in simulated SFG spectra, such as those obtained from atomistic calculations 28,41,[43][44][45][50][51][52] , is likely to be an important next step in this rapidly moving field, along with consideration of possibly absorptive properties of the potential dependent term. As such a treatment has not been considered in the vast literature on this subject, the existing interpretations of resonantly enhanced nonlinear optical responses from charged interfaces need to be carefully reexamined.…”

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confidence: 99%

Second-order spectral lineshapes from charged interfaces

2017

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Second-order nonlinear spectroscopy has proven to be a powerful tool in elucidating key chemical and structural characteristics at a variety of interfaces. However, the presence of interfacial potentials may lead to complications regarding the interpretation of second harmonic and vibrational sum frequency generation responses from charged interfaces due to mixing of absorptive and dispersive contributions. Here, we examine by means of mathematical modeling how this interaction influences second-order spectral lineshapes. We discuss our findings in the context of reported nonlinear optical spectra obtained from charged water/air and solid/liquid interfaces and demonstrate the importance of accounting for the interfacial potential-dependent χ (3) term in interpreting lineshapes when seeking molecular information from charged interfaces using second-order spectroscopy.

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confidence: 99%

Second-order spectral lineshapes from charged interfaces

2017

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“…Among those, the water/air interface has been the most intensively studied system, both experimentally [18][19][20][21][22][23][24][25][26] and theoretically [11,18,[25][26][27][28][29][30][31][32][33][34][35][36]. However, the interpretation of the experimental SFG spectra of the water/air interface in the spectroscopic range between 3000 and 3600 cm −1 is still a matter of great debate [11,19,22,25,30,34,[36][37][38]. In this regard, theoretical SFG simulations have been employed to assist the interpretation and assignment of the O-H stretch vibrational features in the experimental SFG spectra [11,14,18,27,30,36,38,39].…”

Section: Introductionmentioning

confidence: 99%

“…However, the interpretation of the experimental SFG spectra of the water/air interface in the spectroscopic range between 3000 and 3600 cm −1 is still a matter of great debate [11,19,22,25,30,34,[36][37][38]. In this regard, theoretical SFG simulations have been employed to assist the interpretation and assignment of the O-H stretch vibrational features in the experimental SFG spectra [11,14,18,27,30,36,38,39]. Typically, these simulations include intra-and intermolecular vibrational couplings of O-H stretch modes [40][41][42][43], which strongly affects the speed and time scales of spectral diffusion and alters the SFG response of the O-H stretch frequency [18,22].…”

Section: Introductionmentioning

confidence: 99%

Impact of intermolecular vibrational coupling effects on the sum-frequency generation spectra of the water/air interface

et al. 2019

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We have examined the impact of intermolecular vibrational coupling effects of the O-H stretch modes, as obtained by the surface-specific velocity-velocity correlation function approach, on the simulated sum-frequency generation spectra of the water/air interface. Our study shows that the inclusion of intermolecular coupling effects within the first three water layers, i.e. from the water/air interface up to a distance of 6 Å towards the bulk, is essential to reproduce the experimental SFG spectra. In particular, we find that these intermolecular vibrational contributions to the SFG spectra of the water/air interface are dominated by the coupling between the SFG active interfacial and SFG inactive bulk water molecules. Moreover, we find that most of the intermolecular vibrational contributions to the spectra originate from the coupling between double-donor water molecules only, whereas the remaining contributions originate mainly from the coupling between single-donor and double-donor water molecules.

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“…23,[31][32][33][34] While the conventional SFG measurement detects the square of the second-order nonlinear susceptibility | χ (2) | 2 (hereafter χ (2) is denoted as χ), phase-sensitive 35 or heterodyne-detected 36 vibrational SFG (HD-VSFG) measurement can detect the phase of χ (or the imaginary part of χ, Im[ χ]) besides its amplitude, which enables us to detect the orientation of water molecules at the interface, proton-up or proton-down (H-up or H-down). 37 Several HD-VSFG studies clarified detailed molecular orientation at air/water [38][39][40][41][42][43][44][45][46] and lipid (or surfactant)/water [47][48][49][50][51] interfaces.…”

Section: Introductionmentioning

confidence: 99%

Molecular dynamics study of structure and vibrational spectra at zwitterionoic lipid/aqueous KCl, NaCl, and CaCl2 solution interfaces

Ishiyama

Shirai

Okumura

et al. 2018

The Journal of Chemical Physics

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Molecular dynamics (MD) simulations of KCl, NaCl, and CaCl 2 solution/ dipalmytoylphosphatidylcholine lipid interfaces were performed to analyze heterodyne-detected vibrational sum frequency generation (HD-VSFG) spectra in relation to the interfacial water structure. The present MD simulation well reproduces the experimental spectra and elucidates a specific cation effect on the interfacial structure. The K + , Na + , and Ca 2+ cation species penetrate in the lipid layer more than the anions in this order, due to the electrostatic interaction with negative polar groups of lipid, and the electric double layer between the cations and anions cancels the intrinsic orientation of water at the water/lipid interface. These mechanisms explain the HD-VSFG spectrum of the water/lipid interface and its spectral perturbation by adding the ions. The lipid monolayer reverses the order of surface preference of the cations at the solution/lipid interface from that at the solution/air interface. Published by AIP Publishing. https://doi

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Communication: Vibrational sum-frequency spectrum of the air-water interface, revisited

Abstract: Evidence for a liquid-liquid critical point in supercooled water within the E3B3 model and a possible interpretation of the kink in the homogeneous nucleation line

Cited by 70 publications

References 29 publications

Second-order spectral lineshapes from charged interfaces

Second-order spectral lineshapes from charged interfaces

Impact of intermolecular vibrational coupling effects on the sum-frequency generation spectra of the water/air interface

Molecular dynamics study of structure and vibrational spectra at zwitterionoic lipid/aqueous KCl, NaCl, and CaCl2 solution interfaces

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