Development of atom-centered potentials for efficient and accurate electronic structure modeling of large molecular systems
department or school: Science, Irving K. Barber Faculty of (Okanagan)
department or school: Chemistry, Department of (Okanagan)
data provider: DSpace
degree campus: UBCO
creator: Prasad, Viki Kumar
issued: 2022-01-07T18:47:06Z
issued: 2021
related degree: Doctor of Philosophy - PhD
degree grantor: University of British Columbia
description: Accurate quantum mechanical (QM) modeling of large molecular systems is computationally challenging due to the dramatic increase in the demand for computational resources with increasing system size. To tackle this problem, atom-centered potentials (ACPs) were developed to mitigate the errors of Hartree–Fock (HF) and density-functional theory (DFT) methods, particularly when used with small basis sets. The objective behind developing ACPs for such methods was to improve their accuracy in predicting various molecular properties without impacting their low computational cost. ACPs are optimized one-electron Gaussian-type functions that share the same mathematical form as generally used effective-core potentials, except they do not replace any electrons, making them easily usable with many quantum chemistry software packages. Besides, ACPs allow for a convenient means to simultaneously correct the absence of correlation (or deficiencies in exchange-correlation density functionals), basis set incompleteness, and other shortcomings in HF or DFT methods with small basis sets. The overall research conducted for this dissertation demonstrates the gradual transition from the development of proof-of-concept ACPs to final ACPs with more general applicability. In particular, the final ACPs are presented for ten elements in the first and second rows (H, B, C, N, O, F, Si, P, S, Cl), extending the applicability to various organic and biochemical molecules. The ACP-corrected methods have been shown to predict the target molecular properties with slightly less accuracy than very computationally expensive QM methods but at a much lower computational cost. It is anticipated that the methods presented in this dissertation will assist in applications such as supramolecular host-guest complexation, enzymatic catalysis, drug-target binding, protein folding, and others. This dissertation also contributes towards filling the gap in the literature regarding benchmark data sets by presenting…
aggregated CHO: https://circle.library.ubc.ca/rest/handle/2429/80598
note: DEVELOPMENT OF ATOM-CENTERED POTENTIALS FOR EFFICIENT AND ACCURATE ELECTRONIC STRUCTURE MODELING OF LARGE MOLECULAR SYSTEMS by Viki Kumar Prasad B.Sc., St. Xavier’s College, India, 2014 M.Sc., Indian Institute of Technology Kharagpur, India, 2016 A THESIS SUBMITTED IN PARTIAL FULFILLMENT OF THE REQUIREMENTS FOR THE DEGREE OF DOCTOR OF PHILOSOPHY in The College of Graduate Studies (Chemistry) THE UNIVERSITY OF BRITISH COLUMBIA (Okanagan) December 2021 © Viki Kumar Prasad, 2021 ii The following individuals certify that they have read, and recommend to the College of Graduate Studies for acceptance, a thesis/dissertation entitled: DEVELOPMENT OF ATOM-CENTERED POTENTIALS FOR EFFICIENT AND ACCURATE ELECTRONIC STRUCTURE MODELING OF LARGE MOLECULAR SYSTEMS submitted by Viki Kumar Prasad in partial fulfillment of the requirements of the degree of Doctor of Philosophy. Examining Committee: Prof. Gino A. DiLabio, Irving K. Barber Faculty of Science Supervisor Dr. Alberto Otero-de-la-Roza, University of Oviedo Co-supervisor Dr. Isaac T.S. Li, Irving K. Barber Faculty of Science Supervisory Committee Member Dr. David Jack, Irving K. Barber Faculty of Science Supervisory Committee Member Dr. Joshua Brinkerhoff, School of Engineering University Examiner Prof. Erin Johnson, Dalhousie University External Examiner iii Abstract Accurate quantum mechanical (QM) modeling of large molecular systems is computationally challenging due to the dramatic increase in the demand for computational resources with increasing system size. To tackle this problem, atom-centered potentials (ACPs) were developed to mitigate the errors of Hartree–Fock (HF) and density-functional theory (DFT) methods, particularly when used with small basis sets. The objective behind developing ACPs for such methods was to improve their accuracy in predicting various molecular properties without impacting their low computational cost. ACPs are optimized one-electron Gaussian-type functions that share the same mathematica…
has type: Thesis/Dissertation
date issued: 2022-02
is shown at: 10.14288/1.0406216
language: eng
degree discipline: Chemistry
provider: Vancouver : University of British Columbia Library
publisher: University of British Columbia
rights: Attribution-NonCommercial-NoDerivatives 4.0 International
rights URI: http://creativecommons.org/licenses/by-nc-nd/4.0/
scholar level: Graduate
contributor: DiLabio, Gino
contributor: Otero de la Roza, Alberto
type: Text
identifier URI: http://hdl.handle.net/2429/80598