title: Theory of amorphous ices.
abstract: We derive a phase diagram for amorphous solids and liquid supercooled water and explain why the amorphous solids of water exist in several different forms. Application of large-deviation theory allows us to prepare such phases in computer simulations. Along with nonequilibrium transitions between the ergodic liquid and two distinct amorphous solids, we establish coexistence between these two amorphous solids. The phase diagram we predict includes a nonequilibrium triple point where two amorphous phases and the liquid coexist. Whereas the amorphous solids are long-lived and slowly aging glasses, their melting can lead quickly to the formation of crystalline ice. Further, melting of the higher density amorphous solid at low pressures takes place in steps, transitioning to the lower-density glass before accessing a nonequilibrium liquid from which ice coarsens.
authors.affiliation: Department of Chemistry, University of California, Berkeley, CA 94609.
authors.forename: David T
authors.initials: DT
authors.lastname: Limmer
authors.affiliation: Department of Chemistry, University of California, Berkeley, CA 94609 chandler@berkeley.edu.
authors.forename: David
authors.initials: D
authors.lastname: Chandler
mesh_terms: D003460:Crystallization; D007053:Ice; D008956:Models, Chemical; D056004:Molecular Dynamics Simulation; D044367:Phase Transition; D013696:Temperature; D013997:Time Factors
chemical_list: D007053:Ice
keywords: glass transition; putative liquid-liquid transition