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

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, Shin-ya Koshihara, Kazuyuki Takahashi (), Tadahiko Ishikawa () and R. J. Dwayne Miller ()
Additional contact information
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
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

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: 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.

Date: 2024
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DOI: 10.1038/s41467-024-48529-1

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