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Predicting the phase diagram of titanium dioxide with random search and pattern recognition.

Accepted version
Peer-reviewed

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Type

Article

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Authors

Reinhardt, Aleks 
Pickard, Chris J 

Abstract

Predicting phase stabilities of crystal polymorphs is central to computational materials science and chemistry. Such predictions are challenging because they first require searching for potential energy minima and then performing arduous free-energy calculations to account for entropic effects at finite temperatures. Here, we develop a framework that facilitates such predictions by exploiting all the information obtained from random searches of crystal structures. This framework combines automated clustering, classification and visualisation of crystal structures with machine-learning estimation of their enthalpy and entropy. We demonstrate the framework on the technologically important system of TiO2, which has many polymorphs, without relying on prior knowledge of known phases. We find a number of new phases and predict the phase diagram and metastabilities of crystal polymorphs at 1600 K, benchmarking the results against full free-energy calculations.

Description

Keywords

cond-mat.mtrl-sci, cond-mat.mtrl-sci, physics.app-ph

Journal Title

Phys Chem Chem Phys

Conference Name

Journal ISSN

1463-9076
1463-9084

Volume Title

22

Publisher

Royal Society of Chemistry (RSC)

Rights

All rights reserved
Sponsorship
Engineering and Physical Sciences Research Council (EP/P022596/1)
Engineering and Physical Sciences Research Council (EP/P020259/1)
Swiss National Science Foundation (184408)
Swiss National Science Foundation (Project P2ELP2-184408); EPSRC Tier-2 capital grant EP/P020259/1; EPSRC Grant EP/P022596/1; Royal Society Wolfson Research Merit award