Design, Evolution and Spectroscopic Characterization of de novo Photoenzymes

Triplet energy transfer (EnT) photocatalysis is a powerful mode of reactivity in chemical synthesis that allows access to a wide range of transformations that are not accessible in the ground state. However, achieving high levels of stereocontrol and high quantum efficiencies remains a considerable challenge.

To address these limitations we recently designed the first photoenzymes that operate through triplet energy transfer mechanisms (Nature 2022, 611, 709-714).

These enzymes are oxygen tolerant, can operate under ambient reaction conditions, and achieve exceptionally high levels of stereocontrol in a variety of transformations.

With the mechanistic framework for performing EnT photoenzyme catalysis now established, we are now perfectly positioned to develop a new generation of efficient and selective photo-biocatalysts for a wide variety of valuable processes.

In this studentship, we will apply advanced protein engineering technologies to develop highly proficient photoenzymes for new chemical conversions.

We will subsequently gain a detailed understanding of the catalytic mechanisms and structures of excited state intermediates using state-of-the-art laser pulse experiments and EPR spectroscopy.

This knowledge will subsequently be used to inform the design of future generations of photoenzymes with enhanced functions and properties.