Charge transfer dynamics of adsorbate molecules on metal and semiconductor surfaces relating to fundamental processes in dye-sensitized solar cells

Britton, Andrew James (2013) Charge transfer dynamics of adsorbate molecules on metal and semiconductor surfaces relating to fundamental processes in dye-sensitized solar cells. PhD thesis, University of Nottingham.

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The charge transfer dynamics between adsorbate molecules and surfaces are important for a variety of different technologies but especially for dye-sensitized solar cells. The main aim of this thesis was to study charge transfer between organic molecules and surfaces, especially relating to the situation observed in dye sensitized solar cells.

This broad aim can be split into two distinct research objectives. One of these was to study the charge transfer between a Au (111) surface and a variety of different molecules using synchrotron-based photoemission spectroscopy. Resonant photoemission spectra of a C60 monolayer on Au (111) showed distinctive superspectator features which were not observed for the multilayer or clean gold spectra. These features were determined to be resultant from spectator decay involving electrons transferred from the gold substrate to the adsorbed molecule, either in the ground state or during the timescale of the core-hole lifetime. These features were also found for monolayers of bi-isonicotinic, isonicotinic, nicotinic and picolinic acid on gold, but not for the dye molecule, N3, on gold. This suggests that, although charge transfer occurs between the surface and the ligand molecules that constitute N3, no charge transfer occurs between the N3 dye molecule and the gold.

The other objective was to determine whether the core-hole clock technique, previously only used in photoemission spectroscopy, could be adapted for resonant inelastic x-ray scattering. For this, bi-isonicotinic acid on TiO2 was studied because this system had already been explored using photoemission spectroscopy. The charge transfer times were measured using the relative decrease in the elastic peaks for the LUMO and LUMO+1 photon energies of the multilayer and monolayer. This gave a similar result to the photoemission studies providing more confidence for using this adaptation in situations where photoemission would be impossible, such as buried interfaces.

Item Type: Thesis (University of Nottingham only) (PhD)
Supervisors: O' Shea, J.N.
Beton, P.H.
Keywords: Charge transfer resonant photoemission core-hole clock
Subjects: Q Science > QC Physics > QC170 Atomic physics. Constitution and properties of matter
Faculties/Schools: UK Campuses > Faculty of Science > School of Physics and Astronomy
Item ID: 13459
Depositing User: EP, Services
Date Deposited: 06 Nov 2013 10:24
Last Modified: 17 Dec 2017 14:56

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