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Molecular and Interfacial Calculations of Iron(II) Light Harvesters

Fredin, Lisa A. LU ; Wärnmark, Kenneth LU ; Sundström, Villy LU and Persson, Petter LU (2016) In ChemSusChem 9(7). p.667-675
Abstract

Iron-carbene complexes show considerable promise as earth-abundant light-harvesters, and adsorption onto nanostructured TiO2 is a crucial step for developing solar energy applications. Intrinsic electron injection capabilities of such promising FeII N-heterocyclic complexes (Fe-NHC) to TiO2 are calculated here, and found to correlate well with recent experimental findings of highly efficient interfacial injection. First, we examine the special bonding characteristics of Fe-NHC light harvesters. The excited-state surfaces are examined using density functional theory (DFT) and time-dependent DFT (TD-DFT) to explore relaxed excited-state properties. Finally, by relaxing an Fe-NHC adsorbed on a... (More)

Iron-carbene complexes show considerable promise as earth-abundant light-harvesters, and adsorption onto nanostructured TiO2 is a crucial step for developing solar energy applications. Intrinsic electron injection capabilities of such promising FeII N-heterocyclic complexes (Fe-NHC) to TiO2 are calculated here, and found to correlate well with recent experimental findings of highly efficient interfacial injection. First, we examine the special bonding characteristics of Fe-NHC light harvesters. The excited-state surfaces are examined using density functional theory (DFT) and time-dependent DFT (TD-DFT) to explore relaxed excited-state properties. Finally, by relaxing an Fe-NHC adsorbed on a TiO2 nanocluster, we show favorable injection properties in terms of interfacial energy level alignment and electronic coupling suitable for efficient electron injection of excited electrons from the Fe complex into the TiO2 conduction band on ∼100 fs time scales.

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author
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
density functional theory, photochemistry, potential energy surfaces, quantum chemistry, solar energy
in
ChemSusChem
volume
9
issue
7
pages
9 pages
publisher
John Wiley & Sons
external identifiers
  • scopus:84961705010
  • wos:000374156200003
ISSN
1864-5631
DOI
10.1002/cssc.201600062
language
English
LU publication?
yes
id
4f438e17-b69f-406c-a3b2-d2e9e75f537f
date added to LUP
2016-07-18 14:51:51
date last changed
2017-07-23 05:16:23
@article{4f438e17-b69f-406c-a3b2-d2e9e75f537f,
  abstract     = {<p>Iron-carbene complexes show considerable promise as earth-abundant light-harvesters, and adsorption onto nanostructured TiO<sub>2</sub> is a crucial step for developing solar energy applications. Intrinsic electron injection capabilities of such promising Fe<sup>II</sup> N-heterocyclic complexes (Fe-NHC) to TiO<sub>2</sub> are calculated here, and found to correlate well with recent experimental findings of highly efficient interfacial injection. First, we examine the special bonding characteristics of Fe-NHC light harvesters. The excited-state surfaces are examined using density functional theory (DFT) and time-dependent DFT (TD-DFT) to explore relaxed excited-state properties. Finally, by relaxing an Fe-NHC adsorbed on a TiO<sub>2</sub> nanocluster, we show favorable injection properties in terms of interfacial energy level alignment and electronic coupling suitable for efficient electron injection of excited electrons from the Fe complex into the TiO<sub>2</sub> conduction band on ∼100 fs time scales.</p>},
  author       = {Fredin, Lisa A. and Wärnmark, Kenneth and Sundström, Villy and Persson, Petter},
  issn         = {1864-5631},
  keyword      = {density functional theory,photochemistry,potential energy surfaces,quantum chemistry,solar energy},
  language     = {eng},
  month        = {04},
  number       = {7},
  pages        = {667--675},
  publisher    = {John Wiley & Sons},
  series       = {ChemSusChem},
  title        = {Molecular and Interfacial Calculations of Iron(II) Light Harvesters},
  url          = {http://dx.doi.org/10.1002/cssc.201600062},
  volume       = {9},
  year         = {2016},
}