Detection of a Jahn–Teller mode as an ultrafast fingerprint of spin-transition-induced charge transfer in CoFe Prussian Blue Analogue

Hervé, Marius; Marekha, Bogdan; Mazerat, Sandra; Mallah, Talal; Cammarata, Marco; Matar, Samir F.; Haacke, Stefan; Léonard, Jérémie; Collet, Eric

doi:10.1039/d3ma01072d

Mater. Adv.

2024

DOI: 10.1039/d3ma01072d

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Detection of a Jahn–Teller mode as an ultrafast fingerprint of spin-transition-induced charge transfer in CoFe Prussian Blue Analogue

Marius Hervé,

Bogdan Marekha,

Sandra Mazerat

et al.

Abstract: Photoinduced spin transition is one of the fastest processes occurring in transition-metal-based molecules and materials, reaching down to tens of femtoseconds (1 fs = 10−15 s). The underlying dynamics have...

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Cited by 2 publications

References 64 publications

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From Ultrafast Photoinduced Small Polarons to Cooperative and Macroscopic Charge‐Transfer Phase Transition

Privault,

Hervé,

Godin

et al. 2024

Angewandte Chemie

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We study by femtosecond infrared spectroscopy the ultrafast and persistent photoinduced phase transition of the Rb0.94Mn0.94Co0.06[Fe(CN)6]0.98∙0.2H2O material, induced at room temperature by a single laser shot. This system exhibits a charge‐transfer based phase transition with a 75 K wide thermal hysteresis, centred at room temperature, from the low temperature Mn3+−N−C−Fe2+ tetragonal phase to the high temperature Mn2+−N−C−Fe3+ cubic phase. At room temperature, the photoinduced phase transition is persistent. However, the out‐of‐equilibrium dynamics leading to this phase is multi‐scale. Femtosecond infrared spectroscopy, particularly sensitive to local reorganizations through the evolution of the frequency of the N−C vibration modes with the different characteristic electronic states, reveals that at low laser fluence and on short time scale, the photoexcitation of the Mn3+−N−C−Fe2+ phase creates small charge‐transfer polarons [Mn2+−N−C−Fe3+]* within ≃ 250 fs. The local trapping of photoinduced intermetallic charge‐transfer is characterized by the appearance of a polaronic infrared band, due to the surrounding Mn2+−N−C−Fe2+ species. Above a threshold fluence, when a critical fraction of small CT‐polarons is reached, the macroscopic phase transition to the persistent Mn2+−N−C−Fe3+ cubic phase occurs within ≃ 100 ps. This non‐linear photo‐response results from elastic cooperativity, intrinsic to a switchable lattice and reminiscent of a feedback mechanism.

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From Ultrafast Photoinduced Small Polarons to Cooperative and Macroscopic Charge‐Transfer Phase Transition

Privault,

Hervé,

Godin

et al. 2024

Angewandte Chemie

View full text Add to dashboard Cite

show abstract

From Ultrafast Photoinduced Small Polarons to Cooperative and Macroscopic Charge‐Transfer Phase Transition

Privault,

Hervé,

Godin

et al. 2024

Angew Chem Int Ed

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show abstract

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Detection of a Jahn–Teller mode as an ultrafast fingerprint of spin-transition-induced charge transfer in CoFe Prussian Blue Analogue

Abstract: Photoinduced spin transition is one of the fastest processes occurring in transition-metal-based molecules and materials, reaching down to tens of femtoseconds (1 fs = 10−15 s). The underlying dynamics have...

Cited by 2 publications

References 64 publications

From Ultrafast Photoinduced Small Polarons to Cooperative and Macroscopic Charge‐Transfer Phase Transition

From Ultrafast Photoinduced Small Polarons to Cooperative and Macroscopic Charge‐Transfer Phase Transition

From Ultrafast Photoinduced Small Polarons to Cooperative and Macroscopic Charge‐Transfer Phase Transition

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