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Journal Article

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

MPS-Authors
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Bittmann,  S.
International Max Planck Research School for Ultrafast Imaging & Structural Dynamics (IMPRS-UFAST), Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;

External Resource

https://doi.org/10.1038/s41467-024-48529-1
(Publisher version)

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Fulltext (public)

s41467-024-48529-1.pdf
(Publisher version), 6MB

Supplementary Material (public)

suppl.zip
(Supplementary material), 26MB

Citation

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.


Cite as: https://hdl.handle.net/21.11116/0000-000F-670E-F
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.