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Dynamical Transitions of Supercooled Water in Graphene Oxide Nanopores: Influence of Surface Hydrophilicity

Rajasekaran, M and Ganapathy Ayappa, K (2020) Dynamical Transitions of Supercooled Water in Graphene Oxide Nanopores: Influence of Surface Hydrophilicity. In: Journal of Physical Chemistry B, 124 (23). pp. 4805-4820.

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Official URL: https://doi.org/10.1021/acs.jpcb.0c02052


Molecular dynamics simulations are carried out to explore the dynamical crossover phenomenon in strongly confined and mildly supercooled water in graphene oxide nanopores. Since the extent of hydrophilicity can be varied on graphene oxide surfaces, they offer energetically heterogeneous environments that can potentially modulate the rotational and translational relaxation dynamics of confined water. The influence of the physicochemical nature of the graphene oxide surface on the dynamical transitions is investigated by varying the extent of hydrophobicity on the confining surfaces placed at an intersurface separation of 10 à . Water forms two distinct layers in contact with the graphene oxide surface at this separation. All dynamical quantities show a typical slowing down as the temperature is lowered from 298 to 200 K; however, the nature of the transition is a distinct function of the surface type. Water confined between surfaces consisting of alternating hydrophilic and hydrophobic regions exhibit a strong-to-strong dynamical transition in the diffusion coefficients and rotational relaxation times at a crossover temperature of 237 K and show a fragile-to-strong transition in the α-relaxation time at 238 K. The observed crossover temperature is higher than the freezing point of the SPC/E water model used in this study, indicating that these dynamical transitions can occur with mild supercooling under strong confinement in the absence of bulk-like water. In contrast, water confined in a hydrophilic nanopore shows a single Arrhenius energy barrier over the entire temperature range. Our results indicate that in addition to confinement, the nature of the surface can play a critical role in determining the dynamical transitions for water upon supercooling. Copyright © 2020 American Chemical Society.

Item Type: Journal Article
Publication: Journal of Physical Chemistry B
Publisher: American Chemical Society
Additional Information: The copyright for this article belongs to American Chemical Society.
Keywords: Hydrophilicity; Hydrophobicity; Molecular dynamics; Nanopores; Relaxation time; Supercooling, Crossover temperature; Dynamical transition; Heterogeneous environments; Hydrophilic and hydrophobic; Molecular dynamics simulations; Relaxation dynamics; Rotational relaxations; Surface hydrophilicity, Graphene
Department/Centre: Division of Interdisciplinary Sciences > Centre for Biosystems Science and Engineering
Division of Mechanical Sciences > Chemical Engineering
Date Deposited: 06 Feb 2023 07:16
Last Modified: 06 Feb 2023 07:16
URI: https://eprints.iisc.ac.in/id/eprint/79874

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