Electronic and Structural Dynamics During the Switching of the Photomagnetic Complex [Fe(L222N5)(CN)2]
- Univ. of Rennes, UR1-CNRS, UMR 6251 (France). Inst. of Physics of Rennes
- Univ. of Bordeaux, CNRS, ICMCB, Pessac (France); Lebanese German Univ. (LGU), Jounieh (Lebanon)
- Univ. of Bordeaux, CNRS, ICMCB, Pessac (France)
- SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)
- SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS); Paul Scherrer Inst. (PSI), Villigen (Switzerland). SwissFEL
The [Fe(L222N5)(CN)2] compound, where L222N5 refers to the macrocyclic Schiff-base ligand, 2,13-dimethyl-3,6,9,-12,18-pentaazabicyclo[12.3.1]octadeca-1(18),2,12,14,- 16-pentaene, is a photomagnetic FeII based coordination compound, which undergoes light-induced excited spin-state trapping (LIESST). The low spin state is hexacoordinated and the high spin state heptacoordinated. This system also serves as complex for the design of trinuclear or one-dimensional compounds made of other types of bricks with diverse coordinated metals. In this work, its ultrafast spin-state photoswitching dynamics are studied, by combining femtosecond optical spectroscopy and femtosecond X-ray absorption measurements at the XPP station of the X-ray free-electron laser LCLS. DFT and TD-DFT calculations are used to interpret experimental findings. These studies, performed in the solution phase, show that LIESST in [Fe(L222N5)(CN)2] occurs on the 100 fs timescale under different types of photoexcitation. In addition, coherent oscillations were observed, resulting from the structural dynamics accompanying LIESST, which were recently evidenced in more conventional octahedral FeIIN6 systems.
- Research Organization:
- SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
- Sponsoring Organization:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); French National Research Agency (ANR); French National Center for Scientific Research (CNRS); Brittany Region (France). Doctoral Research Allowances (ARED)
- Grant/Contract Number:
- AC02-76SF00515; ANR-13-BS04-0002 FEMTOMAT; ANR-15-CE32-0004 BioXFEL; PEPS SASLELX; ARED 8925/XFELMAT
- OSTI ID:
- 1457700
- Alternate ID(s):
- OSTI ID: 1410596
- Journal Information:
- Chemistry - A European Journal, Vol. 24, Issue 20; ISSN 0947-6539
- Publisher:
- ChemPubSoc EuropeCopyright Statement
- Country of Publication:
- United States
- Language:
- English
Web of Science
Disentangling Ultrafast Electronic and Structural Dynamics with X-Ray Lasers
|
journal | September 2018 |
Photoselective MLCT to d-d pathways for light-induced excited spin state trapping
|
journal | November 2019 |
Pump–probe experimental methodology at the Linac Coherent Light Source
|
journal | April 2019 |
Resolving the Ultrafast Changes of Chemically Inequivalent Metal–Ligand Bonds in Photoexcited Molecular Complexes with Transient X-ray Absorption Spectroscopy
|
journal | April 2019 |
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