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Article Dans Une Revue Angewandte Chemie International Edition Année : 2021

Exploring Ultrafast Photoswitching Pathways in RbMnFe Prussian Blue Analogue

Résumé

We study by femtosecond optical pump-probe spectroscopy the photoinduced charge transfer (CT) in the RbMnFe Prussian blue analogue. Previous studies evidenced the local nature of the photoinduced Mn Fe → Mn Fe process, occurring within less than 1 ps. Here we show experimentally that two photoswitching pathways exist, depending on the excitation pump wavelength, which is confirmed by band structure calculations. Photoexcitation of α spins corresponds to the Mn(d-d) band, which drives reverse Jahn-Teller distortion through the population of antibonding Mn-N orbitals, and induces CT within ≈190 fs. The process launches coherent lattice torsion during the self-trapping of the CT small-polaron. Photoexcitation of β spins drives intervalence Fe→Mn CT towards non-bonding states and results in a slower dynamic.
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Dates et versions

hal-03330845 , version 1 (01-09-2021)

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Giovanni Azzolina, Hiroko Tokoro, Kenta Imoto, Marie Yoshikiyo, Shin-Ichi Ohkoshi, et al.. Exploring Ultrafast Photoswitching Pathways in RbMnFe Prussian Blue Analogue. Angewandte Chemie International Edition, 2021, 60 (43), pp.23267-23273. ⟨10.1002/anie.202106959⟩. ⟨hal-03330845⟩
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