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On the use and development of advanced computational techniques to determine the properties and behaviour of metastable materials

Jobbins, Samuel A. 2017. On the use and development of advanced computational techniques to determine the properties and behaviour of metastable materials. PhD Thesis, Cardiff University.
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This thesis contains discussions and results pertaining to three distinct pieces of work, all related by an underlying theme: the use and development of computational techniques to discover and characterise novel metastable materials. Zinc oxide is a cheap and abundant material with many potential uses in the electronics and Optics industries. However, its wurtzite ground state structure gives rise to a number of undesirable properties. Thus, knowledge of how to stabilise more useful metastable phases is desirable. To that end, the mechanism of the pressure-induced phase transition between the zincblende and rocksalt polymorphs of the compound was deduced using transition path sampling. Following this, a novel technique combining TPS methods with metadynamics was applied to classify the free-energy landscape relevant to the transition pathway. This provided further information relating to the transition that would have been impossible to determine using path based analyses alone. Water ice exhibits a wealth of structural polymorphism, with at least eighteen phases known to experiment and many more configurations predicted. However, a true understanding of the transition pathways that link these structures remains elusive. Using both metadynamics techniques and a novel procedure known as rotational shooting, attempts to deduce pathways between different phases of ice have been made. The results presented include successful transformations between two crystalline phases of ice and several amorphous phases, as well as the possible elucidation of a novel ice polymorph. Crystal structure prediction remains a challenge in materials science. Using a random structure search technique, eight novel allotropes of carbon and three novel high-pressure polymorphs of zinc oxide have been found and subsequently characterised using density functional theory. Each of the materials displays its own unique array of properties, demonstrating both the variety exhibited by polymorphs of the same material and the ability of random structure prediction techniques to predict such dissimilar materials.

Item Type: Thesis (PhD)
Date Type: Submission
Status: Unpublished
Schools: Chemistry
Subjects: Q Science > QD Chemistry
Date of First Compliant Deposit: 24 April 2018
Last Modified: 16 Apr 2021 15:16

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