Direct observation of photoinduced sequential spin transition in a halogen-bonded hybrid system by complementary ultrafast optical and electron probes.

Autor: Jiang Y; European XFEL, Holzkoppel 4, 22869, Schenefeld, Germany. yifeng.jiang@xfel.eu., Hayes S; Departments of Chemistry and Physics, University of Toronto, 80 St. George St., Toronto, M5S 3H6, ON, Canada., Bittmann S; Max Planck Institute for the Structure and Dynamics of Matter, Luruper Chaussee 149, 22761, Hamburg, Germany., Sarracini A; Departments of Chemistry and Physics, University of Toronto, 80 St. George St., Toronto, M5S 3H6, ON, Canada.; Paul Scherrer Institut, Forschungsstrasse 111, 5232, Villigen PSI, Switzerland., Liu LC; Uncharted Software, 600-2 Berkeley St., Toronto, M5A 4J5, ON, Canada., Müller-Werkmeister HM; Institute of Chemistry, University of Potsdam, Karl-Liebknecht-Str. 24-25, 14476, Potsdam-Golm, Germany., Miyawaki A; Department of Chemistry, Graduate School of Science, Kobe University, 1-1, Rokkodai-cho, Nada-ku, Kobe, Hyogo, 657-8501, Japan., Hada M; Tsukuba Research Center for Energy Materials Science, University of Tsukuba, 1-1-1, Tennodai, Tsukuba, Ibaraki, 305-8573, Japan., Nakano S; Department of Chemistry, School of Science, Tokyo Institute of Technology, 2-12-1 Ookayama, Meguro-ku, Tokyo, 152-8551, Japan., Takahashi R; Department of Chemistry, School of Science, Tokyo Institute of Technology, 2-12-1 Ookayama, Meguro-ku, Tokyo, 152-8551, Japan., Banu S; Department of Chemistry, School of Science, Tokyo Institute of Technology, 2-12-1 Ookayama, Meguro-ku, Tokyo, 152-8551, Japan., Koshihara SY; Department of Chemistry, School of Science, Tokyo Institute of Technology, 2-12-1 Ookayama, Meguro-ku, Tokyo, 152-8551, Japan., Takahashi K; Department of Chemistry, Graduate School of Science, Kobe University, 1-1, Rokkodai-cho, Nada-ku, Kobe, Hyogo, 657-8501, Japan. ktaka@crystal.kobe-u.ac.jp., Ishikawa T; Department of Chemistry, School of Science, Tokyo Institute of Technology, 2-12-1 Ookayama, Meguro-ku, Tokyo, 152-8551, Japan. tishi@chem.titech.ac.jp., Miller RJD; Departments of Chemistry and Physics, University of Toronto, 80 St. George St., Toronto, M5S 3H6, ON, Canada. dmiller@lphys2.chem.utoronto.ca.
Jazyk: angličtina
Zdroj: Nature communications [Nat Commun] 2024 Jun 04; Vol. 15 (1), pp. 4604. Date of Electronic Publication: 2024 Jun 04.
DOI: 10.1038/s41467-024-48529-1
Abstrakt: A detailed understanding of the ultrafast dynamics of halogen-bonded materials is desired for designing supramolecular materials and tuning various electronic properties by external stimuli. Here, a prototypical halogen-bonded multifunctional material containing spin crossover (SCO) cations and paramagnetic radical anions is studied as a model system of photo-switchable SCO hybrid systems using ultrafast electron diffraction and two complementary optical spectroscopic techniques. Our results reveal a sequential dynamics from SCO to radical dimer softening, uncovering a key transient intermediate state. In combination with quantum chemistry calculations, we demonstrate the presence of halogen bonds in the low- and high-temperature phases and propose their role during the photoinduced sequential dynamics, underscoring the significance of exploring ultrafast dynamics. Our research highlights the promising utility of halogen bonds in finely tuning functional properties across diverse photoactive multifunctional materials.
(© 2024. The Author(s).)
Databáze: MEDLINE
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