A biomimetic approach for light harvesting using lanthanide binding coiled coils

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Daubney, Oliver James (2019). A biomimetic approach for light harvesting using lanthanide binding coiled coils. University of Birmingham. Ph.D.

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Abstract

Natural inspiration has led to the design and synthesis of a series of novel coiled coil peptides with lanthanide binding sites and chromophores for energy capture and transfer. Their structural and photophysical properties were studied and the complex with the most intense lanthanide emission was explored further as a model system. The use of different chromophores was desired to further expand the lanthanide sensitisation and redox behaviour already exploited by tryptophan. Therefore, a computational methodology for predicting emission spectra from molecular structure was developed. This was validated by comparing the predictions with experimental results for a series of polyaromatic hydrocarbons.

Using the model peptide system a small library of coiled coils was prepared with different chromophores in place of the tryptophan residue. This involved the synthesis of a novel non-natural amino acid and the inclusion of this species in the previously designed sequence. The resulting family of peptides were studied for both their structural and photophysical properties. Throughout this work various novel chromophore to lanthanide interactions have been discovered, expanding the field of energy transfer. This work has led the way for the preparation of a small light harvesting module based upon a coiled coil framework.

Type of Work:

Thesis (Doctorates > Ph.D.)

Award Type:

Doctorates > Ph.D.

Supervisor(s):