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Physical chemistry of gas-phase biological ions; Gas-phase inorganic chemistry; Mass spectrometry

Laser-Interfaced Mass Spectrometry My research interests lie in understanding the fundamental properties of a broad range of photoactive molecules and ensembles. In particular, my focus is on photoactive biological molecules, as well as molecular systems where their photochemical properties can be applied to health problems. My research group employs a novel combination of optical laser spectroscopy along with advanced mass spectrometry techniques. We apply these methods to obtain robust photochemical and photophysical information by examining the systems in the highly-controllable gas-phase environment. Inorganic Metal Complex-Biomolecule Aggregates to Model Photopharmacueticals Photoactivated chemotherapy (PACT) offers both temporal and spatial control over drug activation and has considerable potential for future treatments of cancer. We are investigating metal complex-nucleobase clusters as model systems for identifying fundamental photochemical processes occurring in PACT anti-cancer platinum drug therapies that target DNA. For example, isolated molecular clusters of adenine, cytosine, thymine and uracil bound to hexachloroplatinate, PtCl62-, have been studied using laser electronic photodissociation spectroscopy to investigate photoactivation of a platinum complex in the vicinity of a nucleobase. This is the first study to explore the specific role of a strongly photoactive platinum compound within an aggregate complex. Our results demonstrate how wavelength-dependent selective photoexcitation can drive distinctive photodecay channels (e.g. electron transfer from the metal complex to the nucleobase or proton-abstraction from the nucleobase) for a model photo-pharmaceutical. Such studies provide critical benchmarking data for developing QM/MM methodologies for modelling photoactive metal complex-biomolecule interactions and have the potential to provide a route for facile screening of possible photopharmaceuticals. Current work involves extending these studies to metal-complex-oligonucleotide ensembles.

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