Structure of the water/magnetite interface from sum frequency generation experiments and neural network based molecular dynamics simulations

Fuente: arXiv
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Auteurs principaux: Romano, Salvatore, Kaur, Harsharan, Zelenka, Moritz, De Hijes, Pablo Montero, Eder, Moritz, Parkinson, Gareth S., Backus, Ellen H. G., Dellago, Christoph
Format: Preprint
Publié: 2024
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author Romano, Salvatore
Kaur, Harsharan
Zelenka, Moritz
De Hijes, Pablo Montero
Eder, Moritz
Parkinson, Gareth S.
Backus, Ellen H. G.
Dellago, Christoph
author_facet Romano, Salvatore
Kaur, Harsharan
Zelenka, Moritz
De Hijes, Pablo Montero
Eder, Moritz
Parkinson, Gareth S.
Backus, Ellen H. G.
Dellago, Christoph
contents Magnetite, a naturally abundant mineral, frequently interacts with water in both natural settings and various technical applications, making the study of its surface chemistry highly relevant. In this work, we investigate the hydrogen bonding dynamics and the presence of hydroxyl species at the magnetite-water interface using a combination of neural network potential-based molecular dynamics simulations and sum frequency generation vibrational spectroscopy. Our simulations, which involved large water systems, allowed us to identify distinct interfacial species, such as dissociated hydrogen and hydroxide ions formed by water dissociation. Notably, water molecules near the interface exhibited a preference for dipole orientation towards the surface, with bulk-like water behavior only re-emerging beyond 60 Å from the surface. The vibrational spectroscopy results aligned well with the simulations, confirming the presence of a hydrogen bond network in the surface ad-layers. The analysis revealed that surface-adsorbed hydroxyl groups orient their hydrogen atoms towards the water bulk. In contrast, hydrogen-bonded water molecules align with their hydrogen atoms pointing towards the magnetite surface.
format Preprint
id arxiv_https___arxiv_org_abs_2410_12717
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle Structure of the water/magnetite interface from sum frequency generation experiments and neural network based molecular dynamics simulations
Romano, Salvatore
Kaur, Harsharan
Zelenka, Moritz
De Hijes, Pablo Montero
Eder, Moritz
Parkinson, Gareth S.
Backus, Ellen H. G.
Dellago, Christoph
Materials Science
Chemical Physics
Magnetite, a naturally abundant mineral, frequently interacts with water in both natural settings and various technical applications, making the study of its surface chemistry highly relevant. In this work, we investigate the hydrogen bonding dynamics and the presence of hydroxyl species at the magnetite-water interface using a combination of neural network potential-based molecular dynamics simulations and sum frequency generation vibrational spectroscopy. Our simulations, which involved large water systems, allowed us to identify distinct interfacial species, such as dissociated hydrogen and hydroxide ions formed by water dissociation. Notably, water molecules near the interface exhibited a preference for dipole orientation towards the surface, with bulk-like water behavior only re-emerging beyond 60 Å from the surface. The vibrational spectroscopy results aligned well with the simulations, confirming the presence of a hydrogen bond network in the surface ad-layers. The analysis revealed that surface-adsorbed hydroxyl groups orient their hydrogen atoms towards the water bulk. In contrast, hydrogen-bonded water molecules align with their hydrogen atoms pointing towards the magnetite surface.
title Structure of the water/magnetite interface from sum frequency generation experiments and neural network based molecular dynamics simulations
topic Materials Science
Chemical Physics
url https://arxiv.org/abs/2410.12717