The effect of polymorphism on the structural, dynamic and dielectric properties of plastic crystal water: A molecular dynamics simulation perspective

Abstract

We have employed molecular dynamics simulations based on the TIP4P/2005 water model to investigate the local structural, dynamical, and dielectric properties of the two recently reported body-centered-cubic and face-centered-cubic plastic crystal phases of water. Our results reveal significant differences in the local orientational structure and rotational dynamics of water molecules for the two polymorphs. The probability distributions of trigonal and tetrahedral order parameters exhibit a multi-modal structure, implying the existence of significant local orientational heterogeneities, particularly in the face-centered-cubic phase. The calculated hydrogen bond statistics and dynamics provide further indications of the existence of a strongly heterogeneous and rapidly interconverting local orientational structural network in both polymorphs. We have observed a hindered molecular rotation, much more pronounced in the body-centered-cubic phase, which is reflected by the decay of the fourth-order Legendre reorientational correlation functions and angular Van Hove functions. Molecular rotation, however, is additionally hindered in the high-pressure liquid compared to the plastic crystal phase. The results obtained also reveal significant differences in the dielectric properties of the polymorphs due to the different dipolar orientational correlation characterizing each phase.

References in corpus (10)

• Dynamics of the rotational degrees of freedom in a supercooled liquid of diatomic molecules
• Relation between Rotational and Translational Dynamic Heterogeneities in Water
• The phase diagram of water at high pressures as obtained by computer simulations of the TIP4P/2005 model: the appearance of a plastic crystal phase
• Navigating at Will on the Water Phase Diagram
• Polar nanoregions in water - a study of the dielectric properties of TIP4P/2005, TIP4P/2005f and TTM3F
• Dynamics in a supercooled liquid of symmetric dumbbells: Reorientational hopping for small molecular elongations
• Cooperativity and Heterogeneity in Plastic Crystals Studied by Nonlinear Dielectric Spectroscopy
• Nonlinear dielectric spectroscopy in a fragile plastic crystal
• Water confined in self-assembled ionic surfactants nano-structures
• Structure and dynamics of liquid CS2: Going from ambient to elevated pressure conditions

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