The purported square ice in bilayer graphene is a nanoscale, monolayer object

Pascal, Tod A.; Schwartz, Craig P.; Lawler, Keith V.; Prendergast, David

doi:10.1063/1.5109468

Title: The purported square ice in bilayer graphene is a nanoscale, monolayer object

Journal Article · 18 June 2019 · Journal of Chemical Physics

DOI: https://doi.org/10.1063/1.5109468 · OSTI ID:1546948

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Univ. of California San Diego, La Jolla, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Univ. of Nevada, Las Vegas, NV (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

The phase diagram of water is complex, and interfacial effects can stabilize unusual structures at the nanoscale. In this paper, 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. Finally, simulated core-level spectroscopy reveals unambiguous orientation dependent signatures of square ice that should be discernable in experiments.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC02-76SF00515; AC02-05CH11231; NA0001982; EERE Bridge Project No. 25860

OSTI ID:: 1546948

Alternate ID(s):: OSTI ID: 1526787

Journal Information:: Journal of Chemical Physics, Vol. 150, Issue 23; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 7 works

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