期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 59, 期 1, 页码 364-372出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201908065
关键词
femtochemistry; molecular dynamics; photochemistry; photophysics; X-ray spectroscopy
资金
- Crafoord Foundation
- Knut and Alice Wallenberg Foundation (KAW)
- Swedish Research Council (VR)
- Swedish Energy Agency (Energimyndigheten)
- Swedish Foundation for Strategic Research (SSF)
- Trygger Foundation
- DANSCATT
- Independent Research Fund Denmark [DFF-400200272, DFF-8021-00347B]
- Icelandic Research Fund [196279051]
- Helmholtz Recognition Award
- ELI-ALPS project [GINOP-2.3.615-2015-00001]
- European Union
- European Regional Development Fund [VEKOP-2.3.2-16-201700015]
- Lendglet (Momentum) Program of the Hungarian Academy of Sciences [LP2013-59]
- Government of Hungary
- National Research, Development and Innovation Fund [NKFIH FK 124460]
- U.S. Department of Energy, Office of Science, Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division
- Knut and Alice Wallenberg Foundation [KAW2014.0370]
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-76SF00515]
Iron N-heterocyclic carbene (NHC) complexes have received a great deal of attention recently because of their growing potential as light sensitizers or photocatalysts. We present a sub-ps X-ray spectroscopy study of an (FeNHC)-N-II complex that identifies and quantifies the states involved in the deactivation cascade after light absorption. Excited molecules relax back to the ground state along two pathways: After population of a hot (MLCT)-M-3 state, from the initially excited (MLCT)-M-1 state, 30% of the molecules undergo ultrafast (150 fs) relaxation to the (MC)-M-3 state, in competition with vibrational relaxation and cooling to the relaxed (MLCT)-M-3 state. The relaxed (MLCT)-M-3 state then decays much more slowly (7.6 ps) to the (MC)-M-3 state. The (MC)-M-3 state is rapidly (2.2 ps) deactivated to the ground state. The (MC)-M-5 state is not involved in the deactivation pathway. The ultrafast partial deactivation of the (MLCT)-M-3 state constitutes a loss channel from the point of view of photochemical efficiency and highlights the necessity to screen transition-metal complexes for similar ultrafast decays to optimize photochemical performance.
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