期刊
CHEMICAL SCIENCE
卷 8, 期 7, 页码 4978-4986出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c6sc05624e
关键词
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资金
- Institut Universitaire de France
- Rennes Metropole
- ANR [ANR-13-BS04-0002]
- Centre National de la Recherche Scientifique (CNRS)
- Fonds Europeen de Developpement Regional (FEDER)
- Region Bretagne [ARED 8925/XFELMAT]
- European Research Council (ERC) under the European Union [648558]
Light-induced excited spin state trapping (LIESST) in Fe-II spin-crossover systems is a process that involves the switching of molecules from low (LS, S = 0) to high spin (HS, S = 2) states. The direct LS-to-HS conversion is forbidden by selection rules, and LIESST involves intermediate states such as (MLCT)-M-1,3 or T-1,T-3. The intersystem crossing sequence results in an HS state, structurally trapped by metal-ligand bond elongation through the coherent activation and damping of molecular breathing. The ultrafast dynamics of this process has been investigated in FeN6 ligand field systems, under MLCT excitation. Herein, we studied LIESST in an (FeN4O2)-N-II spin-crossover material of lower symmetry, which allowed for quite intense and low-energy shifted d-d bands. By combining ab initio DFT and TD-DFT calculations and fs optical absorption measurements, we demonstrated that shorter intermediates enhanced coherent structural dynamics, and d-d excitation induced faster LS-to-HS switching, compared to MLCT.
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