Structural and configurational properties of nanoconfined monolayer ice from first principles

Abstract

Understanding the structural tendencies of nanoconfined water is of great interest for nanoscience and biology, where nano/micro-sized objects may be separated by very few layers of water. Here we investigate the properties of ice confined to a quasi-2D monolayer by a featureless, chemically neutral potential, in order to characterize its intrinsic behaviour. We use density-functional theory simulations with a non-local van der Waals density functional. An ab initio random structure search reveals all the energetically competitive monolayer configurations to belong to only two of the previously-identified families, characterized by a square or honeycomb hydrogen-bonding network, respectively. We discuss the modified ice rules needed for each network, and propose a simple point dipole 2D lattice model that successfully explains the energetics of the square configurations. All identified stable phases for both networks are found to be non-polar (but with a topologically non-trivial texture for the square) and, hence, non-ferroelectric, in contrast to previous predictions from a five-site empirical force-field model. Our results are in good agreement with very recently reported experimental observations.

12 pages, 8 figures

References in corpus (23)

• Van der Waals Density Functional for General Geometries
• Maximally-localized generalized Wannier functions for composite energy bands
• Wannier90: A Tool for Obtaining Maximally-Localised Wannier Functions
• Numerical atomic orbitals for linear scaling
• Square ice in graphene nanocapillaries
• A molecular perspective of water at metal interfaces
• What ice can teach us about water interactions: a critical comparison of the performance of different water models
• Effect of pressure on the phase behavior and structure of water confined between nanoscale hydrophobic and hydrophilic plates
• Systematic generation of finite-range atomic basis sets for linear-scaling calculations
• Density, structure and dynamics of water: the effect of Van der Waals interactions
• Thermodynamics, Structure, and Dynamics of Water Confined between Hydrophobic Plates
• 2D ice from first principles: structures and phase transitions
• Nature of the anomalies in the supercooled liquid state of the mW model of water
• Anomalous Nuclear Quantum Effects in Ice
• Electromelting of Confined Monolayer Ice
• Decomposition and terapascal phases of water ice
• New ultrahigh pressure phases of H2O ice predicted using an adaptive genetic algorithm
• Theory of amorphous ices
• Effect of water-wall interaction potential on the properties of nanoconfined water
• Room temperature compressibility and diffusivity of liquid water from first principles
• Enhanced configurational entropy in high-density nanoconfined bilayer ice
• Optimal finite-range atomic basis sets for liquid water and ice
• Band selection and disentanglement using maximally-localized Wannier functions: the cases of Co impurities in bulk copper and the Cu (111) surface

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• Continuous melting through a hexatic phase in confined bilayer water
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• Simulations of water nano-confined between corrugated planes
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