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Probing Transient Valence Orbital Changes with Picosecond Valence-to-Core X-ray Emission Spectroscopy

MPG-Autoren
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Britz,  Alexander
International Max Planck Research School for Ultrafast Imaging & Structural Dynamics (IMPRS-UFAST), Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
European XFEL, Holzkoppel 4, D-22869 Schenefeld, Germany;
The Hamburg Centre for Ultrafast Imaging, Luruper Chaussee 149, 22761 Hamburg, Germany;

Externe Ressourcen

https://doi.org/10.1021/acs.jpcc.6b12940
(Verlagsversion)

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acs.jpcc.6b12940.pdf
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Zitation

March, A. M., Assefa, T. A., Boemer, C., Bressler, C., Britz, A., Diez, M., et al. (2017). Probing Transient Valence Orbital Changes with Picosecond Valence-to-Core X-ray Emission Spectroscopy. The Journal of Physical Chemistry C, 121(5), 2620-2626. doi:10.1021/acs.jpcc.6b12940.


Zitierlink: https://hdl.handle.net/11858/00-001M-0000-002D-7DAE-9
Zusammenfassung
We probe the dynamics of valence electrons in photoexcited [Fe(terpy)2]2+ in solution to gain deeper insight into the Fe–ligand bond changes. We use hard X-ray emission spectroscopy (XES), which combines element specificity and high penetration with sensitivity to orbital structure, making it a powerful technique for molecular studies in a wide variety of environments. A picosecond-time-resolved measurement of the complete 1s X-ray emission spectrum captures the transient photoinduced changes and includes the weak valence-to-core (vtc) emission lines that correspond to transitions from occupied valence orbitals to the nascent core-hole. Vtc-XES offers particular insight into the molecular orbitals directly involved in the light-driven dynamics; a change in the metal–ligand orbital overlap results in an intensity reduction and a blue energy shift in agreement with our theoretical calculations and more subtle features at the highest energies reflect changes in the frontier orbital populations.