The interface of SrTiO3 and H2O from density functional theory molecular dynamics

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The interface of SrTiO3 and H2O from density functional theory molecular dynamics. / Holmström, E.; Spijker, P.; Foster, A. S.

In: PROCEEDINGS OF THE ROYAL SOCIETY A: MATHEMATICAL PHYSICAL AND ENGINEERING SCIENCES, Vol. 472, No. 2193, 20160293, 01.09.2016.

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@article{9b689ad8b5074fc6933dad3cfc28f34f,
title = "The interface of SrTiO3 and H2O from density functional theory molecular dynamics",
abstract = "We use dispersion-corrected density functional theory molecular dynamics simulations to predict the ionic, electronic and vibrational properties of the SrTiO3/H2O solid-liquid interface. Approximately 50{\%} of surface oxygens on the planar SrO termination are hydroxylated at all studied levels of water coverage, the corresponding number being 15{\%} for the planar TiO2 termination and 5{\%} on the stepped TiO2-terminated surface. The lateral ordering of the hydration structure is largely controlled by covalentlike surface cation to H2O bonding and surface corrugation. We find a featureless electronic density of states in and around the band gap energy region at the solid-liquid interface. The vibrational spectrum indicates redshifting of the O-H stretching band due to surface-to-liquid hydrogen bonding and blueshifting due to high-frequency stretching vibrations of OH fragments within the liquid, as well as strong suppression of the OH stretching band on the stepped surface. We find highly varying rates of proton transfer above different SrTiO3 surfaces, owing to differences in hydrogen bond strength and the degree of dissociation of incident water. Trends in proton dynamics and the mode of H2O adsorption among studied surfaces can be explained by the differential ionicity of the Ti-O and Sr-O bonds in the SrTiO3 crystal.",
keywords = "Density functional theory, Hydration structure, Molecular dynamics, Strontium titanate",
author = "E. Holmstr{\"o}m and P. Spijker and Foster, {A. S.}",
year = "2016",
month = "9",
day = "1",
doi = "10.1098/rspa.2016.0293",
language = "English",
volume = "472",
journal = "PROCEEDINGS OF THE ROYAL SOCIETY A: MATHEMATICAL PHYSICAL AND ENGINEERING SCIENCES",
issn = "1364-5021",
number = "2193",

}

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TY - JOUR

T1 - The interface of SrTiO3 and H2O from density functional theory molecular dynamics

AU - Holmström, E.

AU - Spijker, P.

AU - Foster, A. S.

PY - 2016/9/1

Y1 - 2016/9/1

N2 - We use dispersion-corrected density functional theory molecular dynamics simulations to predict the ionic, electronic and vibrational properties of the SrTiO3/H2O solid-liquid interface. Approximately 50% of surface oxygens on the planar SrO termination are hydroxylated at all studied levels of water coverage, the corresponding number being 15% for the planar TiO2 termination and 5% on the stepped TiO2-terminated surface. The lateral ordering of the hydration structure is largely controlled by covalentlike surface cation to H2O bonding and surface corrugation. We find a featureless electronic density of states in and around the band gap energy region at the solid-liquid interface. The vibrational spectrum indicates redshifting of the O-H stretching band due to surface-to-liquid hydrogen bonding and blueshifting due to high-frequency stretching vibrations of OH fragments within the liquid, as well as strong suppression of the OH stretching band on the stepped surface. We find highly varying rates of proton transfer above different SrTiO3 surfaces, owing to differences in hydrogen bond strength and the degree of dissociation of incident water. Trends in proton dynamics and the mode of H2O adsorption among studied surfaces can be explained by the differential ionicity of the Ti-O and Sr-O bonds in the SrTiO3 crystal.

AB - We use dispersion-corrected density functional theory molecular dynamics simulations to predict the ionic, electronic and vibrational properties of the SrTiO3/H2O solid-liquid interface. Approximately 50% of surface oxygens on the planar SrO termination are hydroxylated at all studied levels of water coverage, the corresponding number being 15% for the planar TiO2 termination and 5% on the stepped TiO2-terminated surface. The lateral ordering of the hydration structure is largely controlled by covalentlike surface cation to H2O bonding and surface corrugation. We find a featureless electronic density of states in and around the band gap energy region at the solid-liquid interface. The vibrational spectrum indicates redshifting of the O-H stretching band due to surface-to-liquid hydrogen bonding and blueshifting due to high-frequency stretching vibrations of OH fragments within the liquid, as well as strong suppression of the OH stretching band on the stepped surface. We find highly varying rates of proton transfer above different SrTiO3 surfaces, owing to differences in hydrogen bond strength and the degree of dissociation of incident water. Trends in proton dynamics and the mode of H2O adsorption among studied surfaces can be explained by the differential ionicity of the Ti-O and Sr-O bonds in the SrTiO3 crystal.

KW - Density functional theory

KW - Hydration structure

KW - Molecular dynamics

KW - Strontium titanate

UR - http://www.scopus.com/inward/record.url?scp=84988872479&partnerID=8YFLogxK

U2 - 10.1098/rspa.2016.0293

DO - 10.1098/rspa.2016.0293

M3 - Article

VL - 472

JO - PROCEEDINGS OF THE ROYAL SOCIETY A: MATHEMATICAL PHYSICAL AND ENGINEERING SCIENCES

JF - PROCEEDINGS OF THE ROYAL SOCIETY A: MATHEMATICAL PHYSICAL AND ENGINEERING SCIENCES

SN - 1364-5021

IS - 2193

M1 - 20160293

ER -

ID: 8712957