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Using optical molecular control to explore electronic symmetry and structure.
(LCLS, SLAC National Accelerator Laboratory, USA)
Of the many functional molecular compounds in biology and chemistry, aromaticity seems to play an integral role. Jahn-Teller and similar electronically induced molecular distortions play crucial roles from photo-chemistry to novel superconductivity. In this talk, we will discuss a variational experimental paradigm aimed at combining the electronic sensitivity of normal and resonant Auger x-ray spectroscopies, the structural precision of MeV electron diffraction, and the optical activity of transient absorption spectroscopy. After an overview of the concept, we will see an initial case of correlating these disparate experimental paradigms with the Pseudo-Jahn-Teller system NNO which serves as a linear analogue of the aromatic molecules to come. With this analogue system, we have recently used enhanced molecular rotational coherence to correlate angle dependent Auger electron spectra together with ultrafast MeV scale electron diffraction along with the optical polarizability of NNO. We will finish the discussion with a view of how x-ray pulse shaping in the time-domain can further be applied to such a correlation analysis to better understand the link between molecular structure and chemical function.