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, G. 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, Thomas J. Penfold

Research output: Contribution to journalArticle

3 Citations (Scopus)

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.

Original languageEnglish
Article number3606
JournalNature communications
Volume10
Issue number1
DOIs
Publication statusPublished - Dec 1 2019

Fingerprint

Phenanthrolines
X ray absorption
X ray spectroscopy
Spectrum Analysis
X-Rays
Chemical reactions
spectroscopy
chemical reactions
Potential energy surfaces
x rays
Bond length
Relaxation processes
Excited states
sensitivity
molecular relaxation
breathing
electronics
X rays
Respiration
degrees of freedom

ASJC Scopus subject areas

  • Chemistry(all)
  • Biochemistry, Genetics and Molecular Biology(all)
  • Physics and Astronomy(all)

Cite this

Tracking multiple components of a nuclear wavepacket in photoexcited Cu(I)-phenanthroline complex using ultrafast X-ray spectroscopy. / Katayama, Tetsuo; Northey, Thomas; Gawelda, Wojciech; Milne, Christopher J.; Vankó, G.; Lima, Frederico A.; Bohinc, Rok; Németh, Zoltán; Nozawa, Shunsuke; Sato, Tokushi; Khakhulin, Dmitry; Szlachetko, Jakub; Togashi, Tadashi; Owada, Shigeki; Adachi, Shin ichi; Bressler, Christian; Yabashi, Makina; Penfold, Thomas J.

In: Nature communications, Vol. 10, No. 1, 3606, 01.12.2019.

Research output: Contribution to journalArticle

Katayama, T, Northey, T, Gawelda, W, Milne, CJ, Vankó, G, Lima, FA, Bohinc, R, Németh, Z, Nozawa, S, Sato, T, Khakhulin, D, Szlachetko, J, Togashi, T, Owada, S, Adachi, SI, Bressler, C, Yabashi, M & Penfold, TJ 2019, 'Tracking multiple components of a nuclear wavepacket in photoexcited Cu(I)-phenanthroline complex using ultrafast X-ray spectroscopy', Nature communications, vol. 10, no. 1, 3606. https://doi.org/10.1038/s41467-019-11499-w
Katayama, Tetsuo ; Northey, Thomas ; Gawelda, Wojciech ; Milne, Christopher J. ; Vankó, G. ; Lima, Frederico A. ; Bohinc, Rok ; Németh, Zoltán ; Nozawa, Shunsuke ; Sato, Tokushi ; Khakhulin, Dmitry ; Szlachetko, Jakub ; Togashi, Tadashi ; Owada, Shigeki ; Adachi, Shin ichi ; Bressler, Christian ; Yabashi, Makina ; Penfold, Thomas J. / Tracking multiple components of a nuclear wavepacket in photoexcited Cu(I)-phenanthroline complex using ultrafast X-ray spectroscopy. In: Nature communications. 2019 ; Vol. 10, No. 1.
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