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Kim, Jonggoo
나노물질 및 화학반응 연구단
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Mapping the emergence of molecular vibrations mediating bond formation

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Title
Mapping the emergence of molecular vibrations mediating bond formation
Author(s)
Jong Goo Kim; Nozawa S.; Hanui Kim; Eun Hyuk Choi; Sato T.; Tae Wu Kim; Kim K.H.; Hosung Ki; Jungmin Kim; Minseo Choi; Yunbeom Lee; Jun Heo; Oang K.Y.; Ichiyanagi K.; Fukaya R.; Lee J.H.; Park J.; Eom I.; Chun S.H.; Kim S.; Kim M.; Katayama T.; Togashi T.; Owada S.; Yabashi M.; Sang Jin Lee; Seonggon Lee; Chi Woo Ahn; Doo-Sik Ahn; Moon J.; Choi S.; Kim J.; Joo T.; Kim J.; Adachi S.-I.; Hyotcherl Ihee
Publication Date
2020-06
Journal
NATURE, v.582, no.7813, pp.520 - 524
Publisher
NATURE PUBLISHING GROUP
Abstract
Fundamental studies of chemical reactions often consider the molecular dynamics along a reaction coordinate using a calculated or suggested potential energy surface1–5. But fully mapping such dynamics experimentally, by following all nuclear motions in a time-resolved manner—that is, the motions of wavepackets—is challenging and has not yet been realized even for the simple stereotypical bimolecular reaction6–8: A–B + C → A + B–C. Here we track the trajectories of these vibrational wavepackets during photoinduced bond formation of the gold trimer complex [Au(CN)2−]3 in an aqueous monomer solution, using femtosecond X-ray liquidography9–12 with X-ray free-electron lasers13,14. In the complex, which forms when three monomers A, B and C cluster together through non-covalent interactions15,16, the distance between A and B is shorter than that between B and C. Tracking the wavepacket in three-dimensional nuclear coordinates reveals that within the first 60 femtoseconds after photoexcitation, a covalent bond forms between A and B to give A–B + C. The second covalent bond, between B and C, subsequently forms within 360 femtoseconds to give a linear and covalently bonded trimer complex A–B–C. The trimer exhibits harmonic vibrations that we map and unambiguously assign to specific normal modes using only the experimental data. In principle, more intense X-rays could visualize the motion not only of highly scattering atoms such as gold but also of lighter atoms such as carbon and nitrogen, which will open the door to the direct tracking of the atomic motions involved in many chemical reactions
URI
https://pr.ibs.re.kr/handle/8788114/8995
DOI
10.1038/s41586-020-2417-3
ISSN
0028-0836
Appears in Collections:
Center for Nanomaterials and Chemical Reactions(나노물질 및 화학반응 연구단) > 1. Journal Papers (저널논문)
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