Journal
NATURE
Volume 518, Issue 7539, Pages 385-389Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/nature14163
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Funding
- X-ray Free Electron Laser Priority Strategic Program of MEXT, Japan
- PRESTO/JST
- Innovative Areas 'Artificial Photosynthesis (AnApple)' from Japan Society for the Promotion of Science [25107527]
- Basic Science Research Program through National Research Foundation of Korea - Ministry of Science, ICT & Future Planning [NRF-2014R1A1A1002511]
- [IBS-R004-G2]
- Ministry of Science, ICT & Future Planning, Republic of Korea [IBS-R004-D1-2015-A00] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
- Grants-in-Aid for Scientific Research [25107527, 26102014] Funding Source: KAKEN
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The making and breaking of atomic bonds are essential processes in chemical reactions. Although the ultrafast dynamics of bond breaking have been studied intensively using time-resolved techniques(1-3),, it is very difficult to study the structural dynamics of bond making, mainly because of its bimolecular nature. It is especially difficult to initiate and follow diffusion-limited bond formation in solution with ultrahigh time resolution. Here we use femtosecond time-resolved X-ray solution scattering to visualize the formation of a gold trimer complex, [Au(CN)(2)(-)](3) in real time without the limitation imposed by slow diffusion. This photoexcited gold trimer, which has weakly bound gold atoms in the ground state(4-6), undergoes a sequence of structural changes, and our experiments probe the dynamics of individual reaction steps, including covalent bond formation, the bent-to-linear transition, bond contraction and tetramer formation with a time resolution of 500 femtoseconds. We also determined the three-dimensional structures of reaction intermediates with sub-angstrom spatial resolution. This work demonstrates that it is possible to track in detail and in real time the structural changes that occur during a chemical reaction in solution using X-ray free-electron lasers' and advanced analysis of time-resolved solution scattering data.
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