We have measured the evolution of the THz spectrum of iron(II) spin crossover compounds within the low-spin/high-spin thermal hysteresis loop in the 0.6–6 THz frequency range. This study enabled to follow both the variations of the refractive optical index and absorption during the spin state transition. Marked absorptions centered ∼2 – 3 THz and ∼5 THz shifting with the spin state are revealed. Our work provides a means to store optically information and to read it out in the THz domain and also offers indications about the structural evolution occurring during the spin state transition.

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. Using density functional theory calculations, we were able to retrieve and to visualize these vibrations in both highspin and low-spin states. In both compounds, Raman spectra

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