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Understanding the distinctive and highly directional nature of halogen bonds is crucial for crystal engineering and studying photoinduced structural deformations, which is key for the development of innovative photo-functional materials.

However, the influence of halogen bonds on the rapid photoinduced changes within supramolecular systems remains largely unexplored due to a lack of experimental techniques that can directly observe the halogen bond in action.

This comprehensive approach allowed for a thorough investigation of the photoinduced change of the states, providing a deeper understanding of the underlying processes and intermediates involved.

Furthermore, to elucidate the role of the halogen bonds in the above-mentioned photoinduced sequential dynamics, the researchers conducted quantum chemistry calculations using the ultrafast electron diffraction results.

Overall, the present results underscore the importance of halogen bonds in the photoinduced dynamics, offering a better understanding of the synergistic spin transition.