Ferroaxial order of the monolayer ice in martyite (2503.14018v2)

Abstract: Ice Ih, the most stable phase of water at ambient pressure, is a stacking of the honeycomb network of water molecules H2O. What if one layer of ice is exfoliated and confined to a two-dimensional (2D) sheet? Martyite Zn3(V2O7)(OH)2 2H2O, a mineral with the honeycomb lattice of H2O in the porous framework, is an ideal system for studying such monolayer ice. Due to the geometrical frustration and 2D nature, H2O molecules are dynamically disordered at room temperature. In this study, we reveal disorder-order transitions of H2O in martyite using single-crystal x-ray diffraction (XRD). The XRD results visualize the formation of hydrogen-bonded toroidal H2O hexamers, leading to the ferroaxial order below 200 K. Combined with the molecular dynamics simulations, we discuss the formation process of the H2O hexamers and how they compromise the molecular arrangement towards lower temperatures. Our results unveil the ground state of monolayer ice, a fundamental knowledge to understand the polymorphism of H2O.