Riley, River;
(2020)
Solutions to solvation: multiphoton ultraviolet liquid-microjet photoelectron spectroscopy of organic chromophores.
Doctoral thesis (Ph.D), UCL (University College London).
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Abstract
Photoactive systems found across nature have inspired many innovative technological advances ranging from mimicking photosynthesis to harvest the energy from the Sun to fluorescent probes that have revolutionised biological imaging. Central to the functionality of these systems is the light-interacting chromophore, responsible for the absorption and transfer of energy. A significant proportion of biological and chemical processes occur in environments in which water is the predominant medium. However, the role an environment has on determining how an organic chromophore responds to ultraviolet light is not well understood on the molecular level. Experimentally, the most direct way of probing the electronic structure of a molecule is through the measurement of electron binding energies using photoelectron spectroscopy. Here, multiphoton ultraviolet photoelectron spectroscopy with a liquid-microjet photoelectron spectrometer is employed to investigate how an environment influences the electronic structure and dynamics of organic chromophores. The work focuses on the chromophore of Green Fluorescent Protein (GFP), which ignited the advent of super-high resolution imaging. Firstly, a newly designed and built recirculating liquid-microjet photoelectron spectrometer is described. A recirculating system is essential for studying samples that are only available in relatively small quantities. The instrument is then benchmarked with an investigation on phenol – a molecular motif of the chromophore of GFP – in an aqueous medium. Subsequently, the effect of solvation on the GFP chromophore, in its deprotonated form, is explored. As liquid-microjet ultraviolet photoelectron spectroscopy is a relatively young field, many challenges have arisen, including those originating from inelastic scattering and reorganisation energies of the solvent and solute. This work begins to unravel their effects on and contribution to photoelectron spectra.
| Type: | Thesis (Doctoral) |
|---|---|
| Qualification: | Ph.D |
| Title: | Solutions to solvation: multiphoton ultraviolet liquid-microjet photoelectron spectroscopy of organic chromophores |
| Event: | UCL (University College London) |
| Open access status: | An open access version is available from UCL Discovery |
| Language: | English |
| Additional information: | Copyright © The Author 2020. Original content in this thesis is licensed under the terms of the Creative Commons Attribution 4.0 International (CC BY 4.0) Licence (https://creativecommons.org/licenses/by/4.0/). Any third-party copyright material present remains the property of its respective owner(s) and is licensed under its existing terms. Access may initially be restricted at the author’s request. |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10091083 |
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