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FRA03 |
Where are the Electrons? New Opportunities for Mapping Local Chemical Interaction Dynamics with Time-resolved Soft X-ray Spectroscopy at FELs | |
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Photochemically activated molecules catalyze chemical reactions, but a molecular-level understanding of how these short-lived and reactive intermediates catalyze reactions has remained elusive. I will discuss how time-resolved soft x-ray spectroscopy at free-electron lasers enables a fundamental understanding of local atomic and intermolecular interactions and their dynamics b on atomic length and time scales of Ångströms and femtoseconds[1]. In a recent application[2], we used femtosecond resonant inelastic x-ray scattering (RIXS) at the LINAC Coherent Light Source (LCLS, Stanford, USA)[3] to probe the reaction dynamics of the benchmark transition-metal complex Fe(CO)5 in solution. This highlights the ability of femtosecond soft x-ray spectroscopy at free-electron lasers to probe frontier-orbital interactions with atom specificity. I will end by discussing how the currently available methodology can be extended towards probing complex biomolecules in physiological conditions[4]. I will show how in particular high-repetition rate x-ray free-electron laser sources such as the planned LCLS-II will enable probing the local chemistry and it dynamical evolution in metalloproteins.
[1] Ph. Wernet. Phys. Chem. Chem. Phys. 13, 16941 (2011). [2] Ph. Wernet et al., Nature, 520, 78-81 (2015). [3] K. Kunnus et al., Rev. Sci. Instrum. 83, 123109 (2012). [4] R. Mitzner et al., J. Phys. Chem. Lett. 4, 3641 (2013). |
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Slides FRA03 [61.138 MB] | |
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