4.8 Article

Luminescence and reactivity of a charge-transfer excited iron complex with nanosecond lifetime

期刊

SCIENCE
卷 363, 期 6424, 页码 249-+

出版社

AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.aau7160

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资金

  1. Danish Council for independent Research [5051-00095A, 8021-00410B]
  2. Carlsberg Foundation
  3. Alexander von Humboldt Foundation
  4. Swedish Foundation for Strategic Research
  5. Swedish Research Council
  6. Swedish Energy Agency
  7. Knut and Alice Wallenberg Foundation
  8. Swedish National Supercomputing Center LUNARC
  9. Swedish National Supercomputing Center NISC via SNIC
  10. LMK Foundation
  11. Stiftelsen Die Engkvist Byggmastare
  12. Can Try er Foundation
  13. Wenner-Gren Foundation
  14. Crafoord Foundation
  15. Sten K Johnsons Stiftelse
  16. Royal Physiographic Society

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Iron's abundance and rich coordination chemistry are potentially appealing features for photochemical applications. However, the photoexcitable charge-transfer states of most iron complexes are limited by picosecond or subpicosecond deactivation through low-lying metal-centered states, resulting in inefficient electron-transfer reactivity and complete lack of photoluminescence. In this study, we show that octahedral coordination of iron(Ill) by two mono-anionic facial tris-carbene ligands can markedly suppress such deactivation. The resulting complex [Fe(phtmeimb)(2)](+), where phtmeimb is {phenyl[tris(3-methylimidazol-1-ylidene)]borate}(-), exhibits strong, visible, room temperature photoluminescence with a 2.0-nanosecond lifetime and 2% quantum yield via spin-allowed transition from a doublet ligand-to-metal charge-transfer ((LMCT)-L-2) state to the doublet ground state. Reductive and oxidative electron-transfer reactions were observed for the (2)LMCTstate of [Fe(phtmeimb)(2)](+) in bimolecular quenching studies with methylviologen and diphenylamine.

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