Structure and dynamics of water on the forsterite surface

Tingting Liu; Siddharth Gautam; Hsiu Wen Wang; Lawrence M. Anovitz; Eugene Mamontov; Lawrence F. Allard; David R. Cole

doi:10.1039/c8cp05075a

Structure and dynamics of water on the forsterite surface

Tingting Liu, Siddharth Gautam, Hsiu Wen Wang, Lawrence M. Anovitz, Eugene Mamontov, Lawrence F. Allard, David R. Cole

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12 Scopus citations

Abstract

The behavior of water on mineral surfaces is the key to understanding interfacial and chemical reaction processes. Olivine is one of the major rock-forming minerals and its interaction with water is a ubiquitous phenomenon both on Earth's surface and in the subsurface. This work presents a combined study using molecular dynamics (MD) simulations and quasi-elastic neutron scattering (QENS) experiments conducted using three different instruments to study the structure and dynamics of water on the forsterite (Mg-end member of olivine) surface at 270 K. A combination of three different QENS instruments probes dynamical processes occurring across a broad range of time scales (∼1 ps to ∼1 ns in this study). The water structure on the hydroxylated surface is composed of three distinct water layers, transitioning from well-ordered and nearly immobile closest to the surface to a less structured layer. The energies of three motions (including translation and rotation) derived from simulations agree well with the experiments, covering the energy range from a few to hundreds of micro electron volts.

Original language	English
Pages (from-to)	27822-27829
Number of pages	8
Journal	Physical Chemistry Chemical Physics
Volume	20
Issue number	44
DOIs	https://doi.org/10.1039/c8cp05075a
State	Published - 2018

Funding

We want to thank the two anonymous reviewers whose comments greatly improve the quality of the work. This material is based upon work supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences, Geosciences Program (T. L. and S. G. were supported under the grant DESC0006878 to Ohio State University). T. L. also thanks the computing resources provided by the Deep Carbon Observatory cluster hosted by Rensselaer Polytechnic Institute. We acknowledge the support of the National Institute of Standards and Technology, U.S. Department of Commerce, in providing the neutron research facilities used in this work. Access to DCS and HFBS was provided by the Center for High Resolution Neutron Scattering, a partnership between the National Institute of Standards and Technology and the National Science Foundation under Agreement No. DMR-1508249. The neutron scattering experiments at Oak Ridge National Laboratory’s (ORNL) Spallation Neutron Source were supported by the Scientific User Facilities Division, Office of Basic Energy Sciences, the U.S. Department of Energy (DOE).

Funders	Funder number
Division of Chemical Sciences, Geosciences and Biosciences, Geosciences Program	DESC0006878
Office of Basic Energy Sciences
Scientific User Facilities Division
National Science Foundation
U.S. Department of Energy
National Institute of Standards and Technology
U.S. Department of Commerce
Office of Science
Oak Ridge National Laboratory

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abstract = "The behavior of water on mineral surfaces is the key to understanding interfacial and chemical reaction processes. Olivine is one of the major rock-forming minerals and its interaction with water is a ubiquitous phenomenon both on Earth's surface and in the subsurface. This work presents a combined study using molecular dynamics (MD) simulations and quasi-elastic neutron scattering (QENS) experiments conducted using three different instruments to study the structure and dynamics of water on the forsterite (Mg-end member of olivine) surface at 270 K. A combination of three different QENS instruments probes dynamical processes occurring across a broad range of time scales (∼1 ps to ∼1 ns in this study). The water structure on the hydroxylated surface is composed of three distinct water layers, transitioning from well-ordered and nearly immobile closest to the surface to a less structured layer. The energies of three motions (including translation and rotation) derived from simulations agree well with the experiments, covering the energy range from a few to hundreds of micro electron volts.",

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AU - Liu, Tingting

AU - Gautam, Siddharth

AU - Wang, Hsiu Wen

AU - Anovitz, Lawrence M.

AU - Mamontov, Eugene

AU - Allard, Lawrence F.

AU - Cole, David R.

PY - 2018

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AB - The behavior of water on mineral surfaces is the key to understanding interfacial and chemical reaction processes. Olivine is one of the major rock-forming minerals and its interaction with water is a ubiquitous phenomenon both on Earth's surface and in the subsurface. This work presents a combined study using molecular dynamics (MD) simulations and quasi-elastic neutron scattering (QENS) experiments conducted using three different instruments to study the structure and dynamics of water on the forsterite (Mg-end member of olivine) surface at 270 K. A combination of three different QENS instruments probes dynamical processes occurring across a broad range of time scales (∼1 ps to ∼1 ns in this study). The water structure on the hydroxylated surface is composed of three distinct water layers, transitioning from well-ordered and nearly immobile closest to the surface to a less structured layer. The energies of three motions (including translation and rotation) derived from simulations agree well with the experiments, covering the energy range from a few to hundreds of micro electron volts.

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Structure and dynamics of water on the forsterite surface

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