Tracking multiple components of a nuclear wavepacket in photoexcited Cu(I)-phenanthroline complex using ultrafast X-ray spectroscopy
Tetsuo Katayama (),
Thomas Northey,
Wojciech Gawelda,
Christopher J. Milne,
György Vankó,
Frederico A. Lima,
Rok Bohinc,
Zoltán Németh,
Shunsuke Nozawa,
Tokushi Sato,
Dmitry Khakhulin,
Jakub Szlachetko,
Tadashi Togashi,
Shigeki Owada,
Shin-ichi Adachi,
Christian Bressler,
Makina Yabashi and
Thomas J. Penfold ()
Additional contact information
Tetsuo Katayama: Japan Synchrotron Radiation Research Institute
Thomas Northey: Newcastle University
Wojciech Gawelda: European XFEL
Christopher J. Milne: SwissFEL, Paul Scherrer Institut
György Vankó: Hungarian Academy of Sciences
Frederico A. Lima: European XFEL
Rok Bohinc: SwissFEL, Paul Scherrer Institut
Zoltán Németh: Hungarian Academy of Sciences
Shunsuke Nozawa: High Energy Accelerator Research Organization (KEK)
Tokushi Sato: European XFEL
Dmitry Khakhulin: European XFEL
Jakub Szlachetko: Polish Academy of Sciences
Tadashi Togashi: Japan Synchrotron Radiation Research Institute
Shigeki Owada: Japan Synchrotron Radiation Research Institute
Shin-ichi Adachi: High Energy Accelerator Research Organization (KEK)
Christian Bressler: European XFEL
Makina Yabashi: RIKEN SPring-8 Center
Thomas J. Penfold: Newcastle University
Nature Communications, 2019, vol. 10, issue 1, 1-8
Abstract:
Abstract 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.
Date: 2019
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Persistent link: https://EconPapers.repec.org/RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-019-11499-w
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DOI: 10.1038/s41467-019-11499-w
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