Fireflies glow when a molecule called luciferin reacts with oxygen inside their bodies, and this project will work out exactly how that reaction happens so scientists can design brighter, deeper-penetrating light sources for medical imaging. Current bioluminescent imaging tools lose sensitivity in deep tissue because visible light is absorbed by blood and skin. Newer far-red and near-infrared systems exist, but they are dim and limited in colour range. The researchers will combine ultrafast spectroscopy with quantum chemistry calculations to map the electronic states and molecular motions that cause luciferins to lose energy without emitting light, and to understand how luciferase enzymes shift the colour of the glow. This is fundamental science: there is no immediate clinical application. The goal is a molecular-level blueprint for designing bright, multicolour emitters from scratch, rather than relying on trial-and-error tweaks to existing molecules. If successful, the work could eventually lead to imaging systems that track tumours, infections, or gene expression in real time inside living animals without surgery. Similar fundamental studies of bioluminescence chemistry have already turned a firefly’s glow into a standard laboratory tool; this project aims to give researchers a much wider palette of colours and brighter signals for seeing deeper into tissue.
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This research will improve our molecular level understanding of bioluminescence for the rational design of new near-infrared emitters for advanced bioluminescence imaging applications. Bioluminescence is the emission of light by living organisms. It is one of Nature's most spectacular phenomena and continues to challenge those who try to understand it. The yellow-green glow of fireflies is one of the brightest and most beautiful examples of bioluminescence. The biochemical process involves the catalytic oxidation of a small molecule (luciferin) by an enzyme (luciferase) to form an electronically excited oxyluciferin that subsequently relaxes to its ground state by emitting light. Harnessing bioluminescence for imaging applications has revolutionised the biosciences. Bioluminescence imaging is now a standard tool for visualising molecular and cellular processes in vivo. However, more advanced applications are limited by reduced sensitivity in deep tissue arising from the absorption of visible light by blood and tissue. New far-red and near-infrared bioluminescence systems for enhanced sensitivity and resolution in deep tissue have recently become available; however, they are limited by their brightness and narrow spectral range. There is a pressing need for bright, multicolor, far-red and near-infrared emitters. To date, modifications to bioluminescent systems have relied on incremental changes and small library-based approaches. We propose to use a fundamentally new, bottom-up approach. We will use state-of-the-art spectroscopy measurements and quantum chemistry calculations to learn which electronic states and molecular motions of far-red and near-infrared luciferins are important in the competing non-radiative relaxation pathways that reduce the brightness of bioluminescence and we will learn how luciferase enzymes tune the bioluminescence wavelength. We will then use this information to design new, bright bioluminescent emitters for multicolour, far-red and near-infrared bioluminescence imaging.
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