Absolute orientation of water molecules at the neat water surface

Goh, M. Cynthia; Hicks, Janice M.; Kemnitz, Klaus; Pinto, Giuliano; Heinz, Tony F.; Eisenthal, Kenneth B.; Bhattacharyya, Kankan

doi:10.1021/j100329a003

Cited by 161 publications

(163 citation statements)

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“…The maximum probability is at an angle of 120°with the outward surface normal, which qualitatively agrees with the experimental second-harmonic generation results. 19 Most of the ''classical'' simulations studies also agree with our result, [21][22][23]25 although two studies reported a water dipole orientation parallel to the surface. 20,24 The intramolecular O-H bond orientation can be described by an angle variable between the bond and the surface normal in analogy to the dipole moment orientation angle .…”

Section: Molecular Dynamics Simulation Of Water-vapor Interfacesupporting

confidence: 86%

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Ab initio molecular dynamics simulation of liquid water and water–vapor interface

Vassilev¹,

Hartnig²,

Koper³

et al. 2001

The Journal of Chemical Physics

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The results of ab initio molecular dynamics simulations of liquid water and liquid water–vapor interface using the Perdew-Wang 91 (PW91) exchange-correlation functional are presented. The structural and transport properties of liquid water are comparable to the previous results using Becke-Lee-Yang-Parr (BLYP) functional and experimental data. The shape and the position of the first peak in the oxygen–oxygen radial distribution function is in good agreement with the most recent neutron diffraction data. The ab initio molecular dynamics simulation of liquid water–vapor interface, which is the first of its kind, suggests a preferred orientation of the surface water dipole towards the bulk region.

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Section: Molecular Dynamics Simulation Of Water-vapor Interfacesupporting

confidence: 86%

“…The structure of liquid water-vapor interface has been studied quite intensively using experimental 19 or theoretical [20][21][22][23][24][25][26] methods. These studies, however, lead to different conclusions regarding the orientational distributions of the surface water dipole moments.…”

Section: Introductionmentioning

confidence: 99%

Ab initio molecular dynamics simulation of liquid water and water–vapor interface

Vassilev¹,

Hartnig²,

Koper³

et al. 2001

The Journal of Chemical Physics

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“…In the system described here, the SHG signal originates in the nonresonant electric dipolar contribution of the interfacial molecules. The signal response relates to the overall arrangements of the interfacial entities (Fordyce et al, 2001;Goh et al, 1988;Luca et al, 1995) and is proportional to the incident field and the second-order nonlinear susceptibility χ (2) of the interface. When the interface is charged, due to this charge, the static electric field can induce a third-order nonlinear polarization due to the contribution of the thirdorder nonlinear susceptibility χ (3) of the solution (Ong et al, 1992;Zhao et al, 1993).…”

Section: Introductionmentioning

confidence: 99%

Direct molecular-level characterization of different heterogeneous freezing modes on mica – Part 1

Abdelmonem

2017

Atmos. Chem. Phys.

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Abstract. The mechanisms behind heterogeneous ice nucleation are of fundamental importance to the prediction of the occurrence and properties of many cloud types, which influence climate and precipitation. Aerosol particles act as cloud condensation and freezing nuclei. The surface-water interaction of an ice nucleation particle plays a major, not well explored, role in its ice nucleation ability. This paper presents a real-time molecular-level comparison of different freezing modes on the surface of an atmospherically relevant mineral surface (mica) under varying supersaturation conditions using second-harmonic generation spectroscopy. Two sub-deposition nucleation modes were identified (one-and two-stage freezing). The nonlinear signal at the water-mica interface was found to drop following the formation of a thin film on the surface regardless of (1) the formed phase (liquid or ice) and (2) the freezing path (one or two step), indicating similar molecular structuring. The results also revealed a transient phase of ice at water-mica interfaces during freezing, which has a lifetime of around 1 min. Such information will have a significant impact on climate change, weather modification, and the tracing of water in hydrosphere studies.

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“…Random orientation of these water molecules fitted to this data, less the ~25% that are dipole-neutral, would give them a net dipole of about 40% of the H 2 O molecular dipole. Goh et al (1988) also concluded, from the temperature dependence of the SHG, that water molecules are oriented with their dipole moments pointed, on average, into the bulk at the air-water interface. The water molecules hydrogen-bonded to these, lying just under the surface but within the surface monolayer, would tend to reduce this surface polarity.…”

Section: Sum Frequency Generation and Second Harmonic Generation Specmentioning

confidence: 93%

“…Thus overall it is negative (relative to a positive bulk) but where the very outer layer of the interface (next to the gas) is more positive (Goh et al 1988). They report the probability that this outer (gas-facing) positive contribution is due to the almost-free singly-linked water molecules compensating for the negative quadrupole and dipole contributions in the denser part of the surface layer (Kuz'min, 2000).…”

Section: Simulationsmentioning

confidence: 99%

Untitled

2009

WATER

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SummaryThere is considerable disagreement over whether the gas/liquid surface of water is positive due to the presence of surface-active hydrogen ions or negative due to the presence of surface-active hydroxyl ions. Much has been written and many experimental and simulation studies have been undertaken. We critically analyze these studies to establish what is known unambiguously and what assumptions underlie these opposite views. The conclusion reached after this examination is that there is much misunderstanding over the strength of the evidence for hydrogen ions being surface active and less support for the positive surface than generally regarded. The surface of neutral water is negatively charged.

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Absolute orientation of water molecules at the neat water surface

Cited by 161 publications

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Ab initio molecular dynamics simulation of liquid water and water–vapor interface

Ab initio molecular dynamics simulation of liquid water and water–vapor interface

Direct molecular-level characterization of different heterogeneous freezing modes on mica – Part 1

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