Mapping the emergence of molecular vibrations mediating bond formation

Jong Goo Kim, Shunsuke Nozawa, Hanui Kim, Eun Hyuk Choi, Tokushi Sato, Tae Wu Kim, Kyung Hwan Kim, Hosung Ki, Jungmin Kim, Minseo Choi, Yunbeom Lee, Jun Heo, Key Young Oang, Kouhei Ichiyanagi, Ryo Fukaya, Jae Hyuk Lee, Jaeku Park, Intae Eom, Sae Hwan Chun, Sunam Kim, Minseok Kim, Tetsuo Katayama, Tadashi Togashi, Sigeki Owada, Makina Yabashi, Sang Jin Lee, Seonggon Lee, Chi Woo Ahn, Doo-Sik Ahn, Jiwon Moon, Seungjoo Choi, Joonghan Kim, Taiha Joo, Jeongho Kim, Shin-ichi Adachi and Hyotcherl Ihee ()
Additional contact information
Jong Goo Kim: Department of Chemistry, KAIST
Shunsuke Nozawa: Photon Factory, Institute of Materials Structure Science, High Energy Accelerator Research Organization (KEK)
Hanui Kim: Department of Chemistry, KAIST
Eun Hyuk Choi: Department of Chemistry, KAIST
Tokushi Sato: Center for Free-Electron Laser Science (CFEL), Deutsches Elektronen-Synchrotron (DESY)
Tae Wu Kim: Department of Chemistry, KAIST
Kyung Hwan Kim: Pohang University of Science and Technology (POSTECH)
Hosung Ki: Department of Chemistry, KAIST
Jungmin Kim: Department of Chemistry, KAIST
Minseo Choi: Department of Chemistry, KAIST
Yunbeom Lee: Department of Chemistry, KAIST
Jun Heo: Department of Chemistry, KAIST
Key Young Oang: Quantum Optics Division, Korea Atomic Energy Research Institute (KAERI)
Kouhei Ichiyanagi: Photon Factory, Institute of Materials Structure Science, High Energy Accelerator Research Organization (KEK)
Ryo Fukaya: Photon Factory, Institute of Materials Structure Science, High Energy Accelerator Research Organization (KEK)
Jae Hyuk Lee: Pohang Accelerator Laboratory
Jaeku Park: Pohang Accelerator Laboratory
Intae Eom: Pohang Accelerator Laboratory
Sae Hwan Chun: Pohang Accelerator Laboratory
Sunam Kim: Pohang Accelerator Laboratory
Minseok Kim: Pohang Accelerator Laboratory
Tetsuo Katayama: Japan Synchrotron Radiation Research Institute (JASRI)
Tadashi Togashi: Japan Synchrotron Radiation Research Institute (JASRI)
Sigeki Owada: Japan Synchrotron Radiation Research Institute (JASRI)
Makina Yabashi: Japan Synchrotron Radiation Research Institute (JASRI)
Sang Jin Lee: Department of Chemistry, KAIST
Seonggon Lee: Department of Chemistry, KAIST
Chi Woo Ahn: Department of Chemistry, KAIST
Doo-Sik Ahn: Department of Chemistry, KAIST
Jiwon Moon: The Catholic University of Korea
Seungjoo Choi: Inha University
Joonghan Kim: The Catholic University of Korea
Taiha Joo: Pohang University of Science and Technology (POSTECH)
Jeongho Kim: Inha University
Shin-ichi Adachi: Photon Factory, Institute of Materials Structure Science, High Energy Accelerator Research Organization (KEK)
Hyotcherl Ihee: Department of Chemistry, KAIST

Nature, 2020, vol. 582, issue 7813, 520-524

Abstract: 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.

Date: 2020
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DOI: 10.1038/s41586-020-2417-3

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