Publication Date:
2015-02-20
Description:
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, 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, 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 approximately 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.〈br /〉〈span class="detail_caption"〉Notes: 〈/span〉Kim, Kyung Hwan -- Kim, Jong Goo -- Nozawa, Shunsuke -- Sato, Tokushi -- Oang, Key Young -- Kim, Tae Wu -- Ki, Hosung -- Jo, Junbeom -- Park, Sungjun -- Song, Changyong -- Sato, Takahiro -- Ogawa, Kanade -- Togashi, Tadashi -- Tono, Kensuke -- Yabashi, Makina -- Ishikawa, Tetsuya -- Kim, Joonghan -- Ryoo, Ryong -- Kim, Jeongho -- Ihee, Hyotcherl -- Adachi, Shin-ichi -- England -- Nature. 2015 Feb 19;518(7539):385-9. doi: 10.1038/nature14163.〈br /〉〈span class="detail_caption"〉Author address: 〈/span〉1] Center for Nanomaterials and Chemical Reactions, Institute for Basic Science, Daejeon 305-701, South Korea [2] Department of Chemistry, KAIST, Daejeon 305-701, South Korea. ; Institute of Materials Structure Science, High Energy Accelerator Research Organization, 1-1 Oho, Tsukuba, Ibaraki 305-0801, Japan. ; RIKEN SPring-8 Center, Kouto 1-1-1, Sayo, Hyogo 679-5148, Japan. ; Japan Synchrotron Radiation Research Institute, Kouto 1-1-1, Sayo, Hyogo 679-5198, Japan. ; Department of Chemistry, The Catholic University of Korea, Bucheon 420-743, South Korea. ; Department of Chemistry, Inha University, Incheon 402-751, South Korea. ; 1] Institute of Materials Structure Science, High Energy Accelerator Research Organization, 1-1 Oho, Tsukuba, Ibaraki 305-0801, Japan [2] Department of Materials Structure Science, School of High Energy Accelerator Science, The Graduate University for Advanced Studies, 1-1 Oho, Tsukuba, Ibaraki 305-0801, Japan.〈br /〉〈span class="detail_caption"〉Record origin:〈/span〉 〈a href="http://www.ncbi.nlm.nih.gov/pubmed/25693570" target="_blank"〉PubMed〈/a〉
Print ISSN:
0028-0836
Electronic ISSN:
1476-4687
Topics:
Biology
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Chemistry and Pharmacology
,
Medicine
,
Natural Sciences in General
,
Physics
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