Janus-type emission from a cyclometalated iron(III) complex

Although iron is a dream candidate to substitute noble metals in photoactive complexes, realization of emissive and photoactive iron compounds is demanding due to the fast deactivation of their charge-transfer states. Emissive iron compounds are scarce and dual emission has not been observed before....

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Vydáno v:Nature chemistry Ročník 15; číslo 4; s. 468 - 474
Hlavní autoři: Steube, Jakob, Kruse, Ayla, Bokareva, Olga S, Reuter, Thomas, Demeshko, Serhiy, Schoch, Roland, Argüello Cordero, Miguel A, Krishna, Athul, Hohloch, Stephan, Meyer, Franc, Heinze, Katja, Kühn, Oliver, Lochbrunner, Stefan, Bauer, Matthias
Médium: Journal Article
Jazyk:angličtina
Vydáno: England Nature Publishing Group 01.04.2023
Témata:
Carbenes
Catalysis
Charge transfer
Deactivation
Electron transfer
Emission
Emissions
Heavy metals
Iron
Iron compounds
Ligands
Metals
Noble metals
Oxidation
Photoredox catalysis
ISSN:1755-4330, 1755-4349, 1755-4349
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Popis
Shrnutí:Although iron is a dream candidate to substitute noble metals in photoactive complexes, realization of emissive and photoactive iron compounds is demanding due to the fast deactivation of their charge-transfer states. Emissive iron compounds are scarce and dual emission has not been observed before. Here we report the Fe complex [Fe(ImP) ][PF ] (HImP = 1,1'-(1,3-phenylene)bis(3-methyl-1-imidazol-2-ylidene)), showing a Janus-type dual emission from ligand-to-metal charge transfer (LMCT)- and metal-to-ligand charge transfer (MLCT)-dominated states. This behaviour is achieved by a ligand design that combines four N-heterocyclic carbenes with two cyclometalating aryl units. The low-lying π* levels of the cyclometalating units lead to energetically accessible MLCT states that cannot evolve into LMCT states. With a lifetime of 4.6 ns, the strongly reducing and oxidizing MLCT-dominated state can initiate electron transfer reactions, which could constitute a basis for future applications of iron in photoredox catalysis.
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ISSN:1755-4330
1755-4349
1755-4349
DOI:10.1038/s41557-023-01137-w