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Computational characterization of competing energy and electron transfer states in bimetallic donor-acceptor systems for photocatalytic conversion

Fredin, Lisa A. and Persson, Petter LU (2016) In Journal of Chemical Physics 145(10).
Abstract

The rapidly growing interest in photocatalytic systems for direct solar fuel production such as hydrogen generation from water splitting is grounded in the unique opportunity to achieve charge separation in molecular systems provided by electron transfer processes. In general, both photoinduced and catalytic processes involve complicated dynamics that depend on both structural and electronic effects. Here the excited state landscape of metal centered light harvester-catalyst pairs is explored using density functional theory calculations. In weakly bound systems, the interplay between structural and electronic factors involved can be constructed from the various mononuclear relaxed excited states. For this study, supramolecular states of... (More)

The rapidly growing interest in photocatalytic systems for direct solar fuel production such as hydrogen generation from water splitting is grounded in the unique opportunity to achieve charge separation in molecular systems provided by electron transfer processes. In general, both photoinduced and catalytic processes involve complicated dynamics that depend on both structural and electronic effects. Here the excited state landscape of metal centered light harvester-catalyst pairs is explored using density functional theory calculations. In weakly bound systems, the interplay between structural and electronic factors involved can be constructed from the various mononuclear relaxed excited states. For this study, supramolecular states of electron transfer and excitation energy transfer character have been constructed from constituent full optimizations of multiple charge/spin states for a set of three Ru-based light harvesters and nine transition metal catalysts (based on Ru, Rh, Re, Pd, and Co) in terms of energy, structure, and electronic properties. The complete set of combined charge-spin states for each donor-acceptor system provides information about the competition of excited state energy transfer states with the catalytically active electron transfer states, enabling the identification of the most promising candidates for photocatalytic applications from this perspective.

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publication status
published
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in
Journal of Chemical Physics
volume
145
issue
10
publisher
American Institute of Physics
external identifiers
  • scopus:84987729432
  • wos:000383959000021
ISSN
0021-9606
DOI
10.1063/1.4962254
language
English
LU publication?
yes
id
cebccb6c-5b1d-40aa-8bac-56b0c2c546ac
date added to LUP
2016-11-04 10:15:01
date last changed
2017-09-03 05:14:36
@article{cebccb6c-5b1d-40aa-8bac-56b0c2c546ac,
  abstract     = {<p>The rapidly growing interest in photocatalytic systems for direct solar fuel production such as hydrogen generation from water splitting is grounded in the unique opportunity to achieve charge separation in molecular systems provided by electron transfer processes. In general, both photoinduced and catalytic processes involve complicated dynamics that depend on both structural and electronic effects. Here the excited state landscape of metal centered light harvester-catalyst pairs is explored using density functional theory calculations. In weakly bound systems, the interplay between structural and electronic factors involved can be constructed from the various mononuclear relaxed excited states. For this study, supramolecular states of electron transfer and excitation energy transfer character have been constructed from constituent full optimizations of multiple charge/spin states for a set of three Ru-based light harvesters and nine transition metal catalysts (based on Ru, Rh, Re, Pd, and Co) in terms of energy, structure, and electronic properties. The complete set of combined charge-spin states for each donor-acceptor system provides information about the competition of excited state energy transfer states with the catalytically active electron transfer states, enabling the identification of the most promising candidates for photocatalytic applications from this perspective.</p>},
  articleno    = {104310},
  author       = {Fredin, Lisa A. and Persson, Petter},
  issn         = {0021-9606},
  language     = {eng},
  month        = {09},
  number       = {10},
  publisher    = {American Institute of Physics},
  series       = {Journal of Chemical Physics},
  title        = {Computational characterization of competing energy and electron transfer states in bimetallic donor-acceptor systems for photocatalytic conversion},
  url          = {http://dx.doi.org/10.1063/1.4962254},
  volume       = {145},
  year         = {2016},
}