Karl Franzens University Graz
Graz University of Technology
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Karl Franzens University Graz | Graz University of Technology |
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Discovery of Excited State Pathways in the Ultrafast Photochemistry of Heavy-Atom Systems The coupled electronic and structural dynamics on excited states are fundamental to photoinduced chemical transformations that underpin processes such as photocatalysis, photovoltaic activity, atmospheric chemistry, and luminescence. Of particular interest is the propensity for certain molecules to undergo ultrafast intersystem crossing, which leads to the formation of triplet species that can significantly influence reaction outcomes. One of the techniques my group employs for investigating excited state dynamics is ultrafast extreme ultraviolet (XUV)/soft X-ray transient absorption spectroscopy,1 where transitions between core and valence orbitals report on the evolution of valence electronic structure with element specificity and exquisite sensitivity to spin and orbital character. In this talk, I will present examples of our recent investigations of excited state electronic and structural dynamics in gas-phase systems3-8 including halogen- and transition metal-containing molecules,2 where ultrafast XUV transient absorption spectroscopy has revealed signatures of previously elusive, short-lived electronic states and has provided evidence for ultrafast intersystem crossing. 3,4 I will conclude my talk by presenting our recent investigations of ultrafast charge and energy transfer between plasmonic metals and molecules towards developing an understanding of the first steps in plasmonic photocatalysis. Close collaboration with theorists performing high-level quantum chemical calculations along with predictions of observables allow detailed interpretation of experimental results. |