Navigating at Will on the Water Phase Diagram

Abstract

Despite the simplicity of its molecular unit, water is a challenging system because of its uniquely rich polymorphism and predicted but yet unconfirmed features. Introducing a novel space of generalized coordinates that capture changes in the topology of the interatomic network, we are able to systematically track transitions among liquid, amorphous and crystalline forms throughout the whole phase diagram of water, including the nucleation of crystals above and below the melting point. Our approach, based on molecular dynamics and enhanced sampling / free energy calculation techniques, is not specific to water and could be applied to very different structural phase transitions, paving the way towards the prediction of kinetic routes connecting polymorphic structures in a range of materials.

References in corpus (4)

• Canonical sampling through velocity-rescaling
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Cited by in corpus (16)

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• Machine learning force fields and coarse-grained variables in molecular dynamics: application to materials and biological systems
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• Non-classical nucleation pathways in stacking-disordered crystals
• Beyond Local Structures In Critical Supercooled Water Through Unsupervised Learning
• Nucleating a Different Coordination in a Crystal under Pressure: A Study of the B1-B2 Transition in NaCl by Metadynamics
• Collective Variables for Conformational Polymorphism in Molecular Crystals
• Ephemeral ice-like local environments in classical rigid models of liquid water
• The effect of polymorphism on the structural, dynamic and dielectric properties of plastic crystal water: A molecular dynamics simulation perspective
• Nucleation rates from small scale atomistic simulations and transition state theory
• Out-of-equilibrium Polymorph Selection in Nanoparticle Freezing
• A critical comparison of general-purpose collective variables for crystal nucleation
• A Generalized Nucleation Theory for Ice Crystallization
• Free energy calculations and unbiased dynamics reveal a continuous liquid-liquid transition in water no man's land