Simulations of chiral ordering of achiral molecules by Density Functional Theory and Monte Carlo

Lin, Haiping (2008) Simulations of chiral ordering of achiral molecules by Density Functional Theory and Monte Carlo. PhD thesis, University of Liverpool.

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Abstract

The self-organization of organic molecules on metal surfaces can play a crucial role in various subjects of science such as electrochemistry and heterogeneous catalysis. However, their practical applications have been suffering from lack of atomic scale understanding of the ordering behavior. Theoretically, however, the description of the self-assembly processes has been limited by the inability of microscopic models to account for the interplay of all elementary processes at realistic temperatures and pressures. In this work, we take the succinate molecules and Cu(1IO) surface as a model system to study the nature of the asymmetric self-assembly behavior of the achiral adsorbates on an achiral surface. In the first step, density-functional theory (DFT) is used to accurately characterize the molecule-surface system on the microscopic level. The obtained energetics is then employed to parameterize a lattice gas Hamiltonian, which subsequently allows to address the mesoscopic ordering behavior at finite temperatures by means of ~v1onte Carlo simulations. Two well-defined ordered structures have appeared in the rvlonte Carlo simulations. The (5 0, 3 2) structure has been confirmed to be the ground state configuration by direct DFT calculations. This structure has not been reported before and it can be the ordering configuration observed in some STrvI experiments. By summing up all the calculations, the nature of the self-organization behavior of succinate molecules on Cu(llO) is attributed to the indirect lateral interactions of the adsorbates. This result may provide a new understanding of designing two dimensional periodic architectures on metal surfaces. Supplied by The British Library - 'The world's knowledge'

Item Type:	Thesis (PhD)
Depositing User:	Symplectic Admin
Date Deposited:	20 Oct 2023 09:24
Last Modified:	20 Oct 2023 09:58
DOI:	10.17638/03174412
Copyright Statement:	Copyright © and Moral Rights for this thesis and any accompanying data (where applicable) are retained by the author and/or other copyright owners. A copy can be downloaded for personal non-commercial research or study, without prior permission or charge
URI:	https://livrepository.liverpool.ac.uk/id/eprint/3174412