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Band-selective dynamics in charge-transfer excited iron carbene complexes

Chábera, Pavel LU ; Fredin, Lisa A. LU ; Kjær, Kasper S. LU ; Rosemann, Nils W. LU ; Lindh, Linnea LU ; Prakash, Om LU ; Liu, Yizhu LU ; Wärnmark, Kenneth LU ; Uhlig, Jens LU and Sundström, Villy LU , et al. (2019) In Faraday Discussions 216(2019). p.191-210
Abstract

Ultrafast dynamics of photoinduced charge transfer processes in light-harvesting systems based on Earth-abundant transition metal complexes are of current interest for the development of molecular devices for solar energy conversion applications. A combination of ultrafast spectroscopy and first principles quantum chemical calculations of a recently synthesized iron carbene complex is used to elucidate the ultrafast excited state evolution processes in these systems with particular emphasis on investigating the underlying reasons why these complexes show promise in terms of significantly extended lifetimes of charge transfer excited states. Together, our results challenge the traditional excited state landscape for iron-based light... (More)

Ultrafast dynamics of photoinduced charge transfer processes in light-harvesting systems based on Earth-abundant transition metal complexes are of current interest for the development of molecular devices for solar energy conversion applications. A combination of ultrafast spectroscopy and first principles quantum chemical calculations of a recently synthesized iron carbene complex is used to elucidate the ultrafast excited state evolution processes in these systems with particular emphasis on investigating the underlying reasons why these complexes show promise in terms of significantly extended lifetimes of charge transfer excited states. Together, our results challenge the traditional excited state landscape for iron-based light harvesting transition metal complexes through radically different ground and excited state properties in alternative oxidation states. This includes intriguing indications of rich band-selective excited state dynamics on ultrafast timescales that are interpreted in terms of excitation energy dependence for excitations into a manifold of charge-transfer states. Some implications of the observed excited state properties and photoinduced dynamics for the utilization of iron carbene complexes for solar energy conversion applications are finally discussed.

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Contribution to journal
publication status
published
subject
in
Faraday Discussions
volume
216
issue
2019
pages
20 pages
publisher
Royal Society of Chemistry
external identifiers
  • scopus:85069002599
ISSN
1359-6640
DOI
10.1039/c8fd00232k
language
English
LU publication?
yes
id
bd77f5be-8094-4683-9ae5-24d87300af39
date added to LUP
2019-07-24 12:27:56
date last changed
2019-08-28 04:57:20
@article{bd77f5be-8094-4683-9ae5-24d87300af39,
  abstract     = {<p>Ultrafast dynamics of photoinduced charge transfer processes in light-harvesting systems based on Earth-abundant transition metal complexes are of current interest for the development of molecular devices for solar energy conversion applications. A combination of ultrafast spectroscopy and first principles quantum chemical calculations of a recently synthesized iron carbene complex is used to elucidate the ultrafast excited state evolution processes in these systems with particular emphasis on investigating the underlying reasons why these complexes show promise in terms of significantly extended lifetimes of charge transfer excited states. Together, our results challenge the traditional excited state landscape for iron-based light harvesting transition metal complexes through radically different ground and excited state properties in alternative oxidation states. This includes intriguing indications of rich band-selective excited state dynamics on ultrafast timescales that are interpreted in terms of excitation energy dependence for excitations into a manifold of charge-transfer states. Some implications of the observed excited state properties and photoinduced dynamics for the utilization of iron carbene complexes for solar energy conversion applications are finally discussed.</p>},
  author       = {Chábera, Pavel and Fredin, Lisa A. and Kjær, Kasper S. and Rosemann, Nils W. and Lindh, Linnea and Prakash, Om and Liu, Yizhu and Wärnmark, Kenneth and Uhlig, Jens and Sundström, Villy and Yartsev, Arkady and Persson, Petter},
  issn         = {1359-6640},
  language     = {eng},
  number       = {2019},
  pages        = {191--210},
  publisher    = {Royal Society of Chemistry},
  series       = {Faraday Discussions},
  title        = {Band-selective dynamics in charge-transfer excited iron carbene complexes},
  url          = {http://dx.doi.org/10.1039/c8fd00232k},
  volume       = {216},
  year         = {2019},
}