Surface Reactivity: beyond Born-Oppenheimer
Lead Research Organisation:
University of Bath
Department Name: Physics
Abstract
For many years, a huge effort in theoretical surface science has been directed towards understanding the processes of making and breaking bonds at surfaces. The aim is not only to be able to predict reaction mechanisms and pathways, but also to understand how to manipulate these pathways to open up new avenues for the control of surface chemical reactions. Most of the current theoretical work in surface reactivity uses ab initio electronic structure calculations based on density functional theory (DFT). Underlying these calculations is the Born-Oppenheimer approximation, in which the electrons always remain in their ground state configuration. However, recent experimental results have clearly demonstrated the significant role of electronic excitations in a wide variety of surface reactions. Standard DFT approaches are clearly inadequate here, but there has, to date, been remarkably little progress in developing methods that go beyond the Born-Oppenheimer approximation. It is our aim in this proposal to establish a theoretical framework that will provide a quantitative understanding of the effects of electronic excitations in surface reactions.
Organisations
People |
ORCID iD |
David Bird (Principal Investigator) |
Publications
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Mizielinski MS
(2007)
Spectrum of electronic excitations due to the adsorption of atoms on metal surfaces.
in The Journal of chemical physics
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Forsblom M
(2007)
Vibrational lifetimes of cyanide and carbon monoxide on noble and transition metal surfaces.
in The Journal of chemical physics
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Mizielinski M
(2008)
Newns-Anderson model of chemicurrents in H/Cu and H/Ag
in Surface Science
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Bird D
(2008)
Electronic excitation in atomic adsorption on metals: A comparison of ab initio and model calculations
in Surface Science
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Luntz AC
(2009)
Comment on "role of electron-hole pair excitations in the dissociative adsorption of diatomic molecules on metal surfaces".
in Physical review letters