Journal
NATURE COMMUNICATIONS
Volume 10, Issue -, Pages -Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/s41467-019-11499-w
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Funding
- EPSRC [EP/R021503/1]
- Leverhulme Trust [RPG-2016-103]
- Lendulet (Momentum) Program of the Hungarian Academy of Sciences [LP2013-59]
- Government of Hungary [VEKOP-2.3.2-16-2017-00015]
- European Regional Development Fund [VEKOP-2.3.2-16-2017-00015]
- National Research, Development and Innovation Fund [NKFIH FK 124460]
- European XFEL
- National Science Center (NCN) in Poland under SONATA BIS 6 grant [2016/22/E/ST4/00543]
- German Cluster of Excellence CUI: Advanced Imaging of Matter (AIM)
- JSPS KAKENHI [JP17H06141, JP19H05782, JP19H04407]
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Disentangling the strong interplay between electronic and nuclear degrees of freedom is essential to achieve a full understanding of excited state processes during ultrafast nonadiabatic chemical reactions. However, the complexity of multi-dimensional potential energy surfaces means that this remains challenging. The energy flow during vibrational and electronic relaxation processes can be explored with structural sensitivity by probing a nuclear wavepacket using femtosecond time-resolved X-ray Absorption Near Edge Structure (TR-XANES). However, it remains unknown to what level of detail vibrational motions are observable in this X-ray technique. Herein we track the wavepacket dynamics of a prototypical [Cu(2,9-dimethyl-1,10-phenanthroline)(2)](+) complex using TR-XANES. We demonstrate that sensitivity to individual wavepacket components can be modulated by the probe energy and that the bond length change associated with molecular breathing mode can be tracked with a sub-Angstrom resolution beyond optical-domain observables. Importantly, our results reveal how state-of-the-art TR-XANES provides deeper insights of ultrafast nonadiabatic chemical reactions.
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