Water Orientation at the Calcite-Water Interface

Hagen Söngen; Simon J. Schlegel; Ygor Morais Jaques; John Tracey; Saman Hosseinpour; Doyk Hwang; Ralf Bechstein; Mischa Bonn; Adam S. Foster; Angelika Kühnle; Ellen H.G. Backus

doi:10.1021/acs.jpclett.1c01729

Water Orientation at the Calcite-Water Interface

Hagen Söngen
, Simon J. Schlegel
, Ygor Morais Jaques
, John Tracey
, Saman Hosseinpour
, Doyk Hwang
, Ralf Bechstein
, Mischa Bonn
, Adam S. Foster
, Angelika Kühnle^*
, Ellen H.G. Backus

^*Corresponding author for this work

Research output: Contribution to journal › Article › Scientific › peer-review

23 Citations (Scopus)

72 Downloads (Pure)

Abstract

Mineral-water interfaces play an important role in many natural as well as technological fields. Fundamental properties of these interfaces are governed by the presence of the interfacial water and its specific structure at the surface. Calcite is particularly interesting as a dominant rock-forming mineral in the earth's crust. Here, we combine atomic force microscopy, sum-frequency generation spectroscopy, and molecular dynamics simulations to determine the position and orientation of the water molecules in the hydration layers of the calcite surface with high resolution. While atomic force microscopy provides detailed information about the position of the water molecules at the interface, sum-frequency generation spectroscopy can deduce the orientation of the water molecules. Comparison of the calcite-water interface to the interfaces of magnesite-water, magnesite-ethanol, and calcite-ethanol reveals a comprehensive picture with opposite water orientations in the first and second layer of the interface, which is corroborated by the molecular dynamics simulations.

Original language	English
Pages (from-to)	7605-7611
Number of pages	7
Journal	Journal of Physical Chemistry Letters
Volume	12
Issue number	31
DOIs	https://doi.org/10.1021/acs.jpclett.1c01729
Publication status	Published - 12 Aug 2021
MoE publication type	A1 Journal article-refereed

Funding

Financial support from the German Research Foundation through grant KU1980/14-1, the European Commission through ERC Starting Grant 336679, and the joint program by DAAD (57313835) and National Research Foundation of Korea (NRF-2016K2A9A2A14912842) is gratefully acknowledged. Y.M.J. was supported by the Academy of Finland (project no. 314862). A.S.F. was supported by the World Premier International Research Center Initiative (WPI), MEXT, Japan. Y.M.J. and J.T. acknowledge the use of the computational resources provided by the Aalto Science-IT project and CSC, Helsinki. We thank Hao Lu for the XPS experiments.

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10.1021/acs.jpclett.1c01729

Water Orientation at the Calcite-Water InterfaceFinal published version, 5.07 MBLicence: CC BY

Cite this

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title = "Water Orientation at the Calcite-Water Interface",

abstract = "Mineral-water interfaces play an important role in many natural as well as technological fields. Fundamental properties of these interfaces are governed by the presence of the interfacial water and its specific structure at the surface. Calcite is particularly interesting as a dominant rock-forming mineral in the earth's crust. Here, we combine atomic force microscopy, sum-frequency generation spectroscopy, and molecular dynamics simulations to determine the position and orientation of the water molecules in the hydration layers of the calcite surface with high resolution. While atomic force microscopy provides detailed information about the position of the water molecules at the interface, sum-frequency generation spectroscopy can deduce the orientation of the water molecules. Comparison of the calcite-water interface to the interfaces of magnesite-water, magnesite-ethanol, and calcite-ethanol reveals a comprehensive picture with opposite water orientations in the first and second layer of the interface, which is corroborated by the molecular dynamics simulations. ",

author = "Hagen S{\"o}ngen and Schlegel, \{Simon J.\} and \{Morais Jaques\}, Ygor and John Tracey and Saman Hosseinpour and Doyk Hwang and Ralf Bechstein and Mischa Bonn and Foster, \{Adam S.\} and Angelika K{\"u}hnle and Backus, \{Ellen H.G.\}",

note = "Funding Information: Financial support from the German Research Foundation through grant KU1980/14-1, the European Commission through ERC Starting Grant 336679, and the joint program by DAAD (57313835) and National Research Foundation of Korea (NRF-2016K2A9A2A14912842) is gratefully acknowledged. Y.M.J. was supported by the Academy of Finland (project no. 314862). A.S.F. was supported by the World Premier International Research Center Initiative (WPI), MEXT, Japan. Y.M.J. and J.T. acknowledge the use of the computational resources provided by the Aalto Science-IT project and CSC, Helsinki. We thank Hao Lu for the XPS experiments. Publisher Copyright: {\textcopyright} 2021 The Authors. Published by American Chemical Society.",

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doi = "10.1021/acs.jpclett.1c01729",

language = "English",

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AU - Söngen, Hagen

AU - Schlegel, Simon J.

AU - Morais Jaques, Ygor

AU - Tracey, John

AU - Hosseinpour, Saman

AU - Hwang, Doyk

AU - Bechstein, Ralf

AU - Bonn, Mischa

AU - Foster, Adam S.

AU - Kühnle, Angelika

AU - Backus, Ellen H.G.

N1 - Funding Information: Financial support from the German Research Foundation through grant KU1980/14-1, the European Commission through ERC Starting Grant 336679, and the joint program by DAAD (57313835) and National Research Foundation of Korea (NRF-2016K2A9A2A14912842) is gratefully acknowledged. Y.M.J. was supported by the Academy of Finland (project no. 314862). A.S.F. was supported by the World Premier International Research Center Initiative (WPI), MEXT, Japan. Y.M.J. and J.T. acknowledge the use of the computational resources provided by the Aalto Science-IT project and CSC, Helsinki. We thank Hao Lu for the XPS experiments. Publisher Copyright: © 2021 The Authors. Published by American Chemical Society.

PY - 2021/8/12

Y1 - 2021/8/12

N2 - Mineral-water interfaces play an important role in many natural as well as technological fields. Fundamental properties of these interfaces are governed by the presence of the interfacial water and its specific structure at the surface. Calcite is particularly interesting as a dominant rock-forming mineral in the earth's crust. Here, we combine atomic force microscopy, sum-frequency generation spectroscopy, and molecular dynamics simulations to determine the position and orientation of the water molecules in the hydration layers of the calcite surface with high resolution. While atomic force microscopy provides detailed information about the position of the water molecules at the interface, sum-frequency generation spectroscopy can deduce the orientation of the water molecules. Comparison of the calcite-water interface to the interfaces of magnesite-water, magnesite-ethanol, and calcite-ethanol reveals a comprehensive picture with opposite water orientations in the first and second layer of the interface, which is corroborated by the molecular dynamics simulations.

AB - Mineral-water interfaces play an important role in many natural as well as technological fields. Fundamental properties of these interfaces are governed by the presence of the interfacial water and its specific structure at the surface. Calcite is particularly interesting as a dominant rock-forming mineral in the earth's crust. Here, we combine atomic force microscopy, sum-frequency generation spectroscopy, and molecular dynamics simulations to determine the position and orientation of the water molecules in the hydration layers of the calcite surface with high resolution. While atomic force microscopy provides detailed information about the position of the water molecules at the interface, sum-frequency generation spectroscopy can deduce the orientation of the water molecules. Comparison of the calcite-water interface to the interfaces of magnesite-water, magnesite-ethanol, and calcite-ethanol reveals a comprehensive picture with opposite water orientations in the first and second layer of the interface, which is corroborated by the molecular dynamics simulations.

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VL - 12

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EP - 7611

JO - Journal of Physical Chemistry Letters

JF - Journal of Physical Chemistry Letters

IS - 31

ER -

Water Orientation at the Calcite-Water Interface

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Molecular resolution at solid-liquid interfaces

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Water Orientation at the Calcite-Water Interface

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