Water structuring at stacked graphene interfaces unveiled by machine-learning molecular dynamics

Fuente: arXiv
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Main Authors: Hou, Dianwei, Horbatenko, Yevhen, Ringe, Stefan, Cho, Minhaeng
Format: Preprint
Published: 2025
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author Hou, Dianwei
Horbatenko, Yevhen
Ringe, Stefan
Cho, Minhaeng
author_facet Hou, Dianwei
Horbatenko, Yevhen
Ringe, Stefan
Cho, Minhaeng
contents The wettability of monolayer and multilayer graphene remains a topic of longstanding debate. Here, we combined first-principles molecular dynamics simulations accelerated with the atomic cluster expansion machine learning interatomic potential to investigate how substrate, graphene layer number, and intercalated water molecules influence graphene's wettability. Simulated vibrational sum-frequency generation (vSFG) spectra revealed that the experimentally observed hydrophilic behavior of monolayer graphene on hydrophilic substrates arose not from wetting transparency, but from signal cancellation induced by intercalated water. Energetic analyses further showed that intercalated water molecules were thermodynamically favorable for monolayer graphene on hydrophilic substrates, but not for multilayer systems, leading to changes in the vSFG response in line with experimental observations. These results offer a mechanistic understanding of graphene-water interactions and have broad implications for the design of graphene-based interfaces and devices.
format Preprint
id arxiv_https___arxiv_org_abs_2508_17685
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Water structuring at stacked graphene interfaces unveiled by machine-learning molecular dynamics
Hou, Dianwei
Horbatenko, Yevhen
Ringe, Stefan
Cho, Minhaeng
Chemical Physics
Optics
The wettability of monolayer and multilayer graphene remains a topic of longstanding debate. Here, we combined first-principles molecular dynamics simulations accelerated with the atomic cluster expansion machine learning interatomic potential to investigate how substrate, graphene layer number, and intercalated water molecules influence graphene's wettability. Simulated vibrational sum-frequency generation (vSFG) spectra revealed that the experimentally observed hydrophilic behavior of monolayer graphene on hydrophilic substrates arose not from wetting transparency, but from signal cancellation induced by intercalated water. Energetic analyses further showed that intercalated water molecules were thermodynamically favorable for monolayer graphene on hydrophilic substrates, but not for multilayer systems, leading to changes in the vSFG response in line with experimental observations. These results offer a mechanistic understanding of graphene-water interactions and have broad implications for the design of graphene-based interfaces and devices.
title Water structuring at stacked graphene interfaces unveiled by machine-learning molecular dynamics
topic Chemical Physics
Optics
url https://arxiv.org/abs/2508.17685