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

Zhang, Minli ; Johnson, Catherine E. ; Ilic, Aleksandra LU orcid ; Schwarz, Jesper LU ; Johansson, Malin B. and Lomoth, Reiner (2023) In Journal of the American Chemical Society 145(35). p.19171-19176
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... (More)

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.

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author
; ; ; ; and
organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Journal of the American Chemical Society
volume
145
issue
35
pages
6 pages
publisher
The American Chemical Society (ACS)
external identifiers
  • pmid:37616472
  • scopus:85169848097
ISSN
0002-7863
DOI
10.1021/jacs.3c05404
language
English
LU publication?
yes
id
4291f916-3098-44c6-94a1-65477a48d9db
date added to LUP
2023-11-02 15:12:48
date last changed
2024-04-19 04:32:24
@article{4291f916-3098-44c6-94a1-65477a48d9db,
  abstract     = {{<p>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 <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 amorphous films of pristine [Fe(III)L<sub>2</sub>]PF<sub>6</sub> (L = [phenyl(tris(3-methylimidazol-2-ylidene))borate]<sup>−</sup>). Excitation of the solid material with visible light leads to ultrafast electron transfer quenching of the <sup>2</sup>LMCT 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.</p>}},
  author       = {{Zhang, Minli and Johnson, Catherine E. and Ilic, Aleksandra and Schwarz, Jesper and Johansson, Malin B. and Lomoth, Reiner}},
  issn         = {{0002-7863}},
  language     = {{eng}},
  number       = {{35}},
  pages        = {{19171--19176}},
  publisher    = {{The American Chemical Society (ACS)}},
  series       = {{Journal of the American Chemical Society}},
  title        = {{High-Efficiency Photoinduced Charge Separation in Fe(III)carbene Thin Films}},
  url          = {{http://dx.doi.org/10.1021/jacs.3c05404}},
  doi          = {{10.1021/jacs.3c05404}},
  volume       = {{145}},
  year         = {{2023}},
}