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Title

The Role of Ligand-Field States in the Ultrafast Photophysical Cycle of the Prototypical Iron(II) Spin-Crossover Compound [Fe(ptz)6](BF4)2

Authors
Marino, Andrea
Servol, Marina
Lorenc, Maciej
Collet, Eric
Published in Angewandte Chemie: International Edition. 2014, vol. 53, no. 15, p. 3863-3867
Abstract Light-induced excited spin state trapping (LIESST) in iron(II) spin-crossover compounds, i.e., the light-induced population of the high-spin (S=2) state below the thermal transition temperature, was discovered thirty years ago. For irradiation into metal-ligand charge transfer (MLCT) bands of the low-spin (S=0) species the acknowledged sequence takes the system from the initially excited 1MLCT to the high-spin state via the 3MLCT state within ~150 fs, thereby bypassing low-lying ligand-field (LF) states. Nevertheless, these play role, as borne out by the observation of LIESST and reverse-LIESST on irradiation directly into the LF bands for systems with only high-energy MLCT states. Herein we elucidate the ultrafast reverse-LIESST pathway by identifying the lowest energy S=1 LF state as intermediate state with a lifetime of 39 ps for the light-induced high-spin to low-spin conversion on irradiation into the spin-allowed LF transition of the high-spin species in the NIR.
Keywords Intersystem crossingLIESSTLigand-field statesSpin crossoverUltrafast spectroscopy
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Other version: http://doi.wiley.com/10.1002/anie.201310884
Structures
Research group Groupe Hauser
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MARINO, Andrea et al. The Role of Ligand-Field States in the Ultrafast Photophysical Cycle of the Prototypical Iron(II) Spin-Crossover Compound [Fe(ptz)6](BF4)2. In: Angewandte Chemie: International Edition, 2014, vol. 53, n° 15, p. 3863-3867. https://archive-ouverte.unige.ch/unige:38562

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Deposited on : 2014-07-08

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