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High-Efficiency Photoinduced Charge Separation in Fe(III)carbene Thin Films.


ABSTRACT: Symmetry-breaking charge separation in molecular materials has attracted increasing attention for optoelectronics based on single-material active layers. To this end, Fe(III) complexes with particularly electron-donating N-heterocyclic carbene ligands offer interesting properties with a 2LMCT excited state capable of oxidizing or reducing the complex in its ground state. In this Communication, we show that the corresponding symmetry-breaking charge separation occurs in amorphous films of pristine [Fe(III)L2]PF6 (L = [phenyl(tris(3-methylimidazol-2-ylidene))borate]-). Excitation of the solid material with visible light leads to ultrafast electron transfer quenching of the 2LMCT excited state, generating Fe(II) and Fe(IV) products with high efficiency. Sub-picosecond charge separation followed by recombination in about 1 ns could be monitored by transient absorption spectroscopy. Photoconductivity measurements of films deposited on microelectrode arrays demonstrated that photogenerated charge carriers can be collected at external contacts.

SUBMITTER: Zhang M 

PROVIDER: S-EPMC10485928 | biostudies-literature | 2023 Sep

REPOSITORIES: biostudies-literature

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High-Efficiency Photoinduced Charge Separation in Fe(III)carbene Thin Films.

Zhang Minli M   Johnson Catherine E CE   Ilic Aleksandra A   Schwarz Jesper J   Johansson Malin B MB   Lomoth Reiner R  

Journal of the American Chemical Society 20230824 35


Symmetry-breaking charge separation in molecular materials has attracted increasing attention for optoelectronics based on single-material active layers. To this end, Fe(III) complexes with particularly electron-donating <i>N</i>-heterocyclic carbene ligands offer interesting properties with a <sup>2</sup>LMCT excited state capable of oxidizing or reducing the complex in its ground state. In this Communication, we show that the corresponding symmetry-breaking charge separation occurs in amorphou  ...[more]

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