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Mapping uncharted territory in ice from zeolite networks to ice structures.


Type

Article

Change log

Authors

Engel, Edgar A 
Anelli, Andrea 
Ceriotti, Michele 
Pickard, Chris J 
Needs, Richard J 

Abstract

Ice is one of the most extensively studied condensed matter systems. Yet, both experimentally and theoretically several new phases have been discovered over the last years. Here we report a large-scale density-functional-theory study of the configuration space of water ice. We geometry optimise 74,963 ice structures, which are selected and constructed from over five million tetrahedral networks listed in the databases of Treacy, Deem, and the International Zeolite Association. All prior knowledge of ice is set aside and we introduce "generalised convex hulls" to identify configurations stabilised by appropriate thermodynamic constraints. We thereby rediscover all known phases (I-XVII, i, 0 and the quartz phase) except the metastable ice IV. Crucially, we also find promising candidates for ices XVIII through LI. Using the "sketch-map" dimensionality-reduction algorithm we construct an a priori, navigable map of configuration space, which reproduces similarity relations between structures and highlights the novel candidates. By relating the known phases to the tractably small, yet structurally diverse set of synthesisable candidate structures, we provide an excellent starting point for identifying formation pathways.

Description

Keywords

0406 Physical Geography and Environmental Geoscience

Journal Title

Nat Commun

Conference Name

Journal ISSN

2041-1723
2041-1723

Volume Title

9

Publisher

Springer Science and Business Media LLC
Sponsorship
Royal Society (WM150023)
Engineering and Physical Sciences Research Council (EP/P022596/1)
Engineering and Physical Sciences Research Council (EP/F032773/1)
Engineering and Physical Sciences Research Council (EP/J017639/1)
Engineering and Physical Sciences Research Council (EP/P034616/1)