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The photoinduced switching of Fe(II)-based spin-crossover complexes fromsinglet to quintet takes place at ultrafast time scales. This a priorispin-forbidden transition triggered numerous time-resolved experiments ofsolvated samples to elucidate the mechanism at play. The involved intermediatestates remain uncertain. We apply ultrafast x-ray spectroscopy in molecularfilms as a method sensitive to spin, electronic, and nuclear degrees offreedom. Combining the progress in molecule synthesis and film growth with theopportunities at x-ray free-electron lasers, we analyze the transient evolutionof the Fe L3 fine structure at room temperature. Our measurements andcalculations indicate the involvement of an Fe triplet intermediate state. Thehigh-spin state saturates at half of the available molecules, limited bymolecule-molecule interaction within the film.

Femtosecond spin-state switching dynamics of spin-crossover molecules condensed in thin films