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

Jiang, Y., Hayes, S., Bittmann, S., Sarracini, A., Liu, L. C., Müller-Werkmeister, H. M., et al. (2024). Direct observation of photoinduced sequential spin transition in a halogen-bonded hybrid system by complementary ultrafast optical and electron probes. Nature Communications, 15(1): 4604. doi:10.1038/s41467-024-48529-1.

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Item Permalink: https://hdl.handle.net/21.11116/0000-000F-670E-F Version Permalink: https://hdl.handle.net/21.11116/0000-000F-670F-E
Genre: Journal Article

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 Creators:
Jiang, Y.1, Author
Hayes, S.2, Author
Bittmann, S.3, 4, Author           
Sarracini, A.2, Author
Liu, L. C.5, Author
Müller-Werkmeister, H. M.6, Author
Miyawaki, A.7, Author
Hada, M.8, Author
Nakano, S.9, Author
Takahashi, R.9, Author
Banu, S.9, Author
Koshihara, S.9, Author
Takahashi, K.7, Author
Ishikawa, T.9, Author
Miller, R. J. D.2, Author
Affiliations:
1European XFEL, ou_persistent22              
2Departments of Chemistry and Physics, University of Toronto, ou_persistent22              
3International Max Planck Research School for Ultrafast Imaging & Structural Dynamics (IMPRS-UFAST), Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_2266714              
4Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_1938288              
5Uncharted Software, ou_persistent22              
6Institute of Chemistry, University of Potsdam, ou_persistent22              
7Department of Chemistry, Graduate School of Science, Kobe University, ou_persistent22              
8Tsukuba Research Center for Energy Materials Science, University of Tsukuba, ou_persistent22              
9Department of Chemistry, School of Science, Tokyo Institute of Technology, ou_persistent22              

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 Abstract: 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.

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Language(s): eng - English
 Dates: 2024-01-192024-05-032024-06-04
 Publication Status: Published online
 Pages: -
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1038/s41467-024-48529-1
 Degree: -

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Project name : This research was supported by the Natural Sciences and Engineering Research Council of Canada, Max Planck Society and the excellence cluster “The Hamburg Center for Ultrafast Imaging–Structure, Dynamics and Control of Matter at the Atomic Scale” of the Deutsche Forschungsgemeinschaft (R.J.D.M.), JSPS KAKENHI Grant Numbers JP18H05208 (M.H., S.K., and T.I.), JP19K05402 (K.T.), and JP21K03427 (T.I.). Y.J. acknowledges the financial support from European XFEL GmbH. We would like to thank Jordan Wenzell (Department of Chemistry, University of Toronto) for help in sample preparation. Open Access funding enabled and organized by Projekt DEAL.
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Title: Nature Communications
  Abbreviation : Nat. Commun.
Source Genre: Journal
 Creator(s):
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Publ. Info: London : Nature Publishing Group
Pages: - Volume / Issue: 15 (1) Sequence Number: 4604 Start / End Page: - Identifier: ISSN: 2041-1723
CoNE: https://pure.mpg.de/cone/journals/resource/2041-1723