Document Type

Article

Publication Date

6-18-2019

Publication Title

The Journal of Chemical Physics

Publisher

AIP Publishing

Volume

150

Issue

23

First page number:

1

Last page number:

7

Abstract

The phase diagram of water is complex, and interfacial effects can stabilize unusual structures at the nanoscale. Here, we employ bond order accelerated molecular dynamics simulations to show that upon encapsulation within bilayer graphene, water can spontaneously adopt a two-dimensional (monomolecular) layer of “square ice” at ambient conditions, instead of an encapsulated water droplet. Free energy calculations show that this motif is thermodynamically stable up to diameters of approximately 15 nm due to enhanced hydrogen bonding and favorable binding to the graphene sheets. Entropic losses due to solidification and reduced graphene–graphene binding enthalpy are opposing thermodynamic forces that conspire to limit the maximum size, but modification of any of these thermodynamic factors should change the range of stability. Simulated core-level spectroscopy reveals unambiguous orientation dependent signatures of square ice that should be discernable in experiments.

Disciplines

Atomic, Molecular and Optical Physics

File Format

pdf

File Size

2.857 KB

Language

English

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