Surface tension of <i>ab initio</i> liquid water at the water-air interface

Nagata, Yuki; Ohto, Tatsuhiko; Bonn, Mischa; Kühne, Thomas D.

doi:10.1063/1.4951710

Cited by 52 publications

(66 citation statements)

References 100 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…For numerical reasons, the intermolecular pair potential in molecular simulation needs to be truncated. However, thermodynamic properties in heterogeneous systems are very sensitive to a truncation of the intermolecular potential [10,11,38,[47][48][49][50][51][52][53][54][55][56]. For the Lennard-Jones potential, a large variety of long-range corrections (LRC) exist for heterogeneous systems to account for the inhomogeneity, ranging from Ewald summation techniques [57][58][59], the Fast Multipole Method (FMM) [60] and Multilevel Summation (MLS) [61] to slab-based LRC techniques [62][63][64].…”

Section: Simulations With the Mie Potentialmentioning

confidence: 99%

Simultaneous description of bulk and interfacial properties of fluids by the Mie potential

et al. 2016

View full text Add to dashboard Cite

The vapor-liquid equilibrium (VLE) of the Mie potential, where the dispersive exponent is constant (m = 6) while the repulsive exponent n is varied between 9 and 48, is systematically investigated by molecular simulation. For systems with planar vapor-liquid interfaces, long-range correction expressions are derived, so that interfacial and bulk properties can be computed accurately. The present simulation results are found to be consistent with the available body of literature on the Mie fluid which is substantially extended. On the basis of correlations for the considered thermodynamic properties, a multicriteria optimization becomes viable. Thereby, users can adjust the three parameters of the Mie potential to the properties of real fluids, weighting different thermodynamic properties according to their importance for a particular application scenario. In the present work, this is demonstrated for carbon dioxide for which different competing objective functions are studied which describe the accuracy of the model for representing the saturated liquid density, the vapor pressure and the surface tension. It is shown that models can be found which describe simultaneously the saturated liquid density and vapor pressure with good accuracy, and it is discussed to what extent this accuracy can be upheld as the model accuracy for the surface tension is further improved.

show abstract

Section: Simulations With the Mie Potentialmentioning

confidence: 99%

Simultaneous description of bulk and interfacial properties of fluids by the Mie potential

et al. 2016

View full text Add to dashboard Cite

show abstract

“…For the more accurate water models, such as polarizable models, even the simple task of structurally relaxing supercooled water can be prohibitively costly. For instance, the timescales accessible to state-ofthe-art ab initio MD simulations do not typically exceed 100 ps [117], which is considerably shorter than the characteristic structural relaxation time of supercooled water computed from typical classical non-polarizable forcefields [118]. This is in addition to the activated nature of ice nucleation, which usually involves crossing large nucleation barriers that can, sometimes, be only overcome by employing advanced sampling techniques.…”

Section: Study Of Homogeneous Ice Nucleationmentioning

confidence: 99%

Perspective: Surface freezing in water: A nexus of experiments and simulations

Haji-Akbari

Debenedetti

2017

The Journal of Chemical Physics

View full text Add to dashboard Cite

Surface freezing is a phenomenon in which crystallization is enhanced at a vapor-liquid interface. In some systems, such as n-alkanes, this enhancement is dramatic, and results in the formation of a crystalline layer at the free interface even at temperatures slightly above the equilibrium bulk freezing temperature. There are, however, systems in which the enhancement is purely kinetic, and only involves faster nucleation at or near the interface. The first, thermodynamic, type of surface freezing is easier to confirm in experiments, requiring only the verification of the existence of crystalline order at the interface. The second, kinetic, type of surface freezing is far more difficult to prove experimentally. One material that is suspected of undergoing the second type of surface freezing is liquid water. Despite strong indications that the freezing of liquid water is kinetically enhanced at vapor-liquid interfaces, the findings are far from conclusive, and the topic remains controversial. In this perspective, we present a simple thermodynamic framework to understand conceptually and distinguish these two types of surface freezing. We then briefly survey fifteen years of experimental and computational work aimed at elucidating the surface freezing conundrum in water.

show abstract

“…36 The choice of BLYP exchange and correlation functionals plus D3 correction arises from the fact that this combination can reproduce both the surface tension 37 and SFG spectra 38 accurately. Furthermore, the absorption energy calculation of water on rutile TiO 2 surface demonstrated that the van der Waals corrections are essential for reproducing the water conformation (molecular vs dissociated state) on the TiO 2 surface.…”

mentioning

confidence: 99%

Chemisorbed and Physisorbed Water at the TiO₂/Water Interface

Hosseinpour

Tang

Wang

et al. 2017

J. Phys. Chem. Lett.

Self Cite

View full text Add to dashboard Cite

The interfacial structure of water in contact with TiO2 is the key to understand the mechanism of photocatalytic water dissociation as well as photoinduced superhydrophilicity. We investigate the interfacial molecular structure of water at the surface of anatase TiO2, using phase-sensitive sum frequency generation spectroscopy together with spectra simulation using ab initio molecular dynamic trajectories. We identify two oppositely oriented, weakly and strongly hydrogen-bonded subensembles of O–H groups at the superhydrophilic UV irradiated TiO2 surface. The water molecules with weakly hydrogen-bonded O–H groups are chemisorbed, i.e. form hydroxyl groups, at the TiO2 surface with their hydrogen atoms pointing toward bulk water. The strongly hydrogen-bonded O–H groups interact with the oxygen atom of the chemisorbed water. Their hydrogen atoms point toward the TiO2. This strong interaction between physisorbed and chemisorbed water molecules causes superhydrophilicity.

show abstract

Surface tension of ab initio liquid water at the water-air interface

Cited by 52 publications

References 100 publications

Simultaneous description of bulk and interfacial properties of fluids by the Mie potential

Simultaneous description of bulk and interfacial properties of fluids by the Mie potential

Perspective: Surface freezing in water: A nexus of experiments and simulations

Chemisorbed and Physisorbed Water at the TiO₂/Water Interface

Contact Info

Product

Resources

About

Surface tension of ab initio liquid water at the water-air interface

Cited by 52 publications

References 100 publications

Simultaneous description of bulk and interfacial properties of fluids by the Mie potential

Simultaneous description of bulk and interfacial properties of fluids by the Mie potential

Perspective: Surface freezing in water: A nexus of experiments and simulations

Chemisorbed and Physisorbed Water at the TiO2/Water Interface

Contact Info

Product

Resources

About

Chemisorbed and Physisorbed Water at the TiO₂/Water Interface