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

Author

Listed:
  • Yifeng Jiang

    (European XFEL)

  • Stuart Hayes

    (University of Toronto)

  • Simon Bittmann

    (Max Planck Institute for the Structure and Dynamics of Matter)

  • Antoine Sarracini

    (University of Toronto
    Paul Scherrer Institut)

  • Lai Chung Liu

    (Uncharted Software)

  • Henrike M. Müller-Werkmeister

    (University of Potsdam)

  • Atsuhiro Miyawaki

    (Kobe University)

  • Masaki Hada

    (University of Tsukuba)

  • Shinnosuke Nakano

    (Tokyo Institute of Technology)

  • Ryoya Takahashi

    (Tokyo Institute of Technology)

  • Samiran Banu

    (Tokyo Institute of Technology)

  • Shin-ya Koshihara

    (Tokyo Institute of Technology)

  • Kazuyuki Takahashi

    (Kobe University)

  • Tadahiko Ishikawa

    (Tokyo Institute of Technology)

  • R. J. Dwayne Miller

    (University of Toronto)

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.

Suggested Citation

  • Yifeng Jiang & Stuart Hayes & Simon Bittmann & Antoine Sarracini & Lai Chung Liu & Henrike M. Müller-Werkmeister & Atsuhiro Miyawaki & Masaki Hada & Shinnosuke Nakano & Ryoya Takahashi & Samiran Banu , 2024. "Direct observation of photoinduced sequential spin transition in a halogen-bonded hybrid system by complementary ultrafast optical and electron probes," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-48529-1
    DOI: 10.1038/s41467-024-48529-1
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    References listed on IDEAS

    as
    1. C. Mariette & M. Lorenc & H. Cailleau & E. Collet & L. Guérin & A. Volte & E. Trzop & R. Bertoni & X. Dong & B. Lépine & O. Hernandez & E. Janod & L. Cario & V. Ta Phuoc & S. Ohkoshi & H. Tokoro & L. , 2021. "Strain wave pathway to semiconductor-to-metal transition revealed by time-resolved X-ray powder diffraction," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
    2. Yifeng Jiang & Lai Chung Liu & Antoine Sarracini & Kamil M. Krawczyk & Jordan S. Wentzell & Cheng Lu & Ryan L. Field & Samir F. Matar & Wojciech Gawelda & Henrike M. Müller-Werkmeister & R. J. Dwayne , 2020. "Direct observation of nuclear reorganization driven by ultrafast spin transitions," Nature Communications, Nature, vol. 11(1), pages 1-8, December.
    3. Henrik T. Lemke & Kasper S. Kjær & Robert Hartsock & Tim B. van Driel & Matthieu Chollet & James M. Glownia & Sanghoon Song & Diling Zhu & Elisabetta Pace & Samir F. Matar & Martin M. Nielsen & Mauriz, 2017. "Coherent structural trapping through wave packet dispersion during photoinduced spin state switching," Nature Communications, Nature, vol. 8(1), pages 1-8, August.
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