Rules essential to water molecular undercoordination

TL;DR

This paper explores the molecular undercoordination in water ice, revealing how it leads to supersolidity, unique physical properties, and anomalies, by analyzing hydrogen bond dynamics and electronic structure.

Contribution

It introduces new concepts linking molecular undercoordination to water's supersolid phase and its anomalous behaviors, advancing understanding of water's core physics.

Findings

Undercoordination shortens HO bonds and stiffens phonons.

Molecular undercoordination causes supersolidity with unique properties.

Water's supersolid skin is hydrophobic and thermally stable.

Abstract

A sequential of concepts developed in last decade has enabled a resolution to multiple anomalies of water ice and its low-dimensionality, particularly. Developed concepts include the coupled hydrogen bond oscillator pair, segmental specific heat, three-body coupling potentials, quasisolidity, and supersolidity. Resolved anomalies include ice buoyancy, ice slipperiness, water skin toughness, supercooling and superheating at the nanoscale, etc. Evidence shows consistently that molecular undercoordination shortens the HO bond and stiffens its phonon while undercoordination does the OH nonbond contrastingly associated with strong lone pair polarization, which endows the low-dimensional water ice with supersolidity. The supersolid phase is hydrophobic, less dense, viscoelastic, thermally more diffusive and stable, having longer electron and phonon lifetime. The equal number of lone pairs and protons reserves the configuration and orientation of the coupled hydrogen bond bonds and restricts molecular rotation and proton hopping, which entitles water the simplest, ordered, tetrahedrally-coordinated, fluctuating molecular crystal covered with a supersolid skin. The hydrogen bond segmental cooperativity and specific-heat disparity form the soul dictating the extraordinary adaptivity, reactivity, recoverability, sensitivity of water ice when subjecting to physical perturbation. It is recommended that the premise of hydrogen bonding and electronic dynamics would deepen the insight into the core physics and chemistry of water ice.