Hill, Adam ORCID: 0000-0001-8503-9219 (2023) On the generation of ab initio potential energy surfaces using machine learning techniques. PhD thesis, University of Sheffield.
Abstract
A potential energy surface is a major pre-requisite to carrying out quantum molecular dynamics studies on chemical systems. These studies allow theoreticians to explore the behaviour of modern-day chemistry in ways that are not feasible in a lab, enabling predictions to be made about experiments performed at extreme temperatures and pressures, and even helping to reveal reaction pathways. To achieve this, a PES associates nuclear position and energy, constructing an n-dimensional surface from high-level ab initio calculations that are fit using physically motivated functions. However, this fitting is a painstakingly slow process, and must be tailored to individual systems. This thesis will explore three ways of speeding up the generation of ab initio PESs: simplifying the fitting process, reducing the number of fitting points, and reducing the computational cost of the ab initio calculations themselves. Machine learning (ML) algorithms offer a number of potential advantages for the construction of PESs: firstly, they represent more of a ``black-box'' approach to the fitting that promises an easier route to accurate surfaces; second, reducing the dimensionality of the problem holds the promise of constructing a surface from significantly fewer points. These algorithms also have access to active learning techniques that aim to reduce the size of machine learning datasets. As such, a particular subset of machine learning model, the neural network, will be used along side a novel application of a firefly inspired optimisation algorithm to speed up PES generation. While the development of new basis sets paired with correlation consistent effective core potentials will aim to speed up data generation.
Metadata
Supervisors: | Hill, J. Grant and Meijer, Anthony J H M |
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Awarding institution: | University of Sheffield |
Academic Units: | The University of Sheffield > Faculty of Science (Sheffield) > Chemistry (Sheffield) |
Depositing User: | Mr Adam Hill |
Date Deposited: | 17 Oct 2023 14:24 |
Last Modified: | 17 Oct 2023 14:24 |
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