Proceedings of September Meeting 2016 (NFM16)
Publication date: 14th June 2016
Over last decades, the transition metal complexes (Pt, Ir and Ru) have received great attention due to their long-lived electronic excited states, for applications such as OLEDs and DSSCs.[1] However, the replacement of these expensive, scarce and toxic metals by earth-abundant metals as Fe or Cu is still extremely changing due to a smaller ligand field splitting. A possible way to stabilize the 3MLCT temporally is by increasing the ligand field strength in order toavoid the 0.1ps spin cross-over into metal-centered high spin states observed in Fe-pyridine complexes[2]. Recently, the use of N-heterocyclic carbenes (NHC) ligands was reported to lead to a prolonged 3MLCT lifetime (9 ps)[3], which we were able to extend up to 16.5ps due to carboxylation of the ligands[4] (fig. A). Very recently, the Wärnmark group working on the same carboxylated complex, reported efficient electron injection into TiO2 by using THz spectroscopy, but also deleterious charge recombination.[5] We have designed new complexes where iron was coordinated by benzimidazolylidene-based (Biz) which affords a new record 3MLCT lifetime of 26 ps in MeCN.[5] Streak camera fluorescence experiments on complexes grafted on TiO2 and Al2O3 substrates indicate electron injection through shorter 3MLCT state lifetime on TiO2 than on high-band gap Al2O3 (fig. B), but also surprisingly long 3MLCT state lifetime components induced only through binding on the semiconductor surfaces. A detailed modeling of the effect of surface attachment on the excited state ordering is in progress.
[1] Chan et al. ACS Nano 2009, 3, 3103.
[2] Consani et al. Angew. Chem., Int. Ed., 2009, 48, 7184
[3] Liu et al. Chem. Comm., 2013, 21, 6412
[4] T. Duchanois, et al., Eur. J. Inorg. Chem. 2015, 14, 2469-2477.
[5] Harlang et al. Nat. Chem.2015,7, 883.
[6] Liu et al. Phys. Chem. Chem. Phys, 2016, 18, 12550
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