Publicly Offered Research
Grant-in-Aid for Scientific Research on Innovative Areas (Research in a proposed research area)
Excited state structural dynamics of transition metal complexes are important not only for applications but also for rethinking the fundamental concepts. Ultrafast spectroscopy is the common method for such studies. However, real-space determination of the structural changes in the excited state remained challenging due to transient nature of the intermediate(S). In this proposal, we aim to use the TR-SFX method for observing structural dynamics of a tetrahedral Cu(I)-phen complex in ultrafast timescale.
We immobilized a light-sensitive Mn-carbonyl complex in the porous lysozyme crystal and characterized by ATR-IR and absorbance spectroscopy. We determined the structure under darkness and compared with metal-free protein. We applied TR-SFX method to determine the changes at the metal reaction center after light irradiation. This gave interesting features such as releasing of CO ligand sequentially and the intermediate in which a water molecule was coordinated. The release of CO ligand was estimated by considering the appearance of negative density features after light irradiation which was were increased with increasing delay time. High laser intensity was found to trigger the CO release reaction. The results were validated by the QM MM calculations.
令和5年度が最終年度であるため、記入しない。
All 2024 2023
All Journal Article (3 results) (of which Int'l Joint Research: 3 results, Peer Reviewed: 3 results, Open Access: 3 results)
Nat. Commun
Volume: 15 Issue: 1 Pages: 5518-5518
10.1038/s41467-024-49814-9
Cryst. Growth Des.
Volume: 23 Issue: 10 Pages: 7448-7458
10.1021/acs.cgd.3c00880
Biomater. Sci.
Volume: 12 Issue: 9 Pages: 2408-2417
10.1039/d4bm00173g
