Giant magnetic field effects in donor–acceptor triads : On the charge separation and recombination dynamics in triarylamine–naphthalenediimide triads with bis-diyprrinato-palladium(II), porphodimethenato-palladium(II), and palladium(II)–porphyrin photosensitizers

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2020
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Riese, Stefan
Brand, Jessica S.
Mims, David
Holzapfel, Marco
Lukzen, Nikita N.
Lambert, Christoph
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The Journal of Chemical Physics. American Institute of Physics (AIP). 2020, 153(5), 054306. ISSN 0021-9606. eISSN 1089-7690. Available under: doi: 10.1063/5.0013941
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A series of triads consisting of a triarylamine donor, a naphthalenediimide acceptor, and a palladium photosensitizer bridge was investigated for the photoinduced electron transfer processes and the spin chemistry involved. In this series, the ligand in the palladium photosensitizer was varied from bis-dipyrrinato to porphodimethenato and to a porphyrin. With the porphyrin photosensitizer, no charge separated state could be reached. This is caused by the direct relaxation of the excited photosensitizer to the ground state by intersystem crossing. The bis-dipyrrinato-palladium photosensitizer gave only a little yield (7%) of the charge separated state, which is due to the population of a metal centered triplet state and a concomitant geometrical rearrangement to a disphenoidal coordination sphere. This state relaxes rapidly to the ground state. In contrast, in the porphodimethenato-palladium triads, a long lived (μs to ms) charge separated state could be generated in high quantum yields (66%–74%) because, here, the population of a triplet metal centered state is inhibited by geometrical constraints. The magnetic field dependent transient absorption measurement of one of the porphodimethenato triads revealed a giant magnetic field effect by a factor of 26 on the signal amplitude of the charge separated state. This is the consequence of a magnetic field dependent triplet–singlet interconversion that inhibits the fast decay of the charge separated triplet state through the singlet recombination channel. A systematic comparative analysis of the spin-dependent kinetics in terms of three classical and one fully quantum theoretical methods is provided, shedding light on the pros and cons of each of them.

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ISO 690RIESE, Stefan, Jessica S. BRAND, David MIMS, Marco HOLZAPFEL, Nikita N. LUKZEN, Ulrich STEINER, Christoph LAMBERT, 2020. Giant magnetic field effects in donor–acceptor triads : On the charge separation and recombination dynamics in triarylamine–naphthalenediimide triads with bis-diyprrinato-palladium(II), porphodimethenato-palladium(II), and palladium(II)–porphyrin photosensitizers. In: The Journal of Chemical Physics. American Institute of Physics (AIP). 2020, 153(5), 054306. ISSN 0021-9606. eISSN 1089-7690. Available under: doi: 10.1063/5.0013941
BibTex
@article{Riese2020-08-07Giant-50676,
  year={2020},
  doi={10.1063/5.0013941},
  title={Giant magnetic field effects in donor–acceptor triads : On the charge separation and recombination dynamics in triarylamine–naphthalenediimide triads with bis-diyprrinato-palladium(II), porphodimethenato-palladium(II), and palladium(II)–porphyrin photosensitizers},
  number={5},
  volume={153},
  issn={0021-9606},
  journal={The Journal of Chemical Physics},
  author={Riese, Stefan and Brand, Jessica S. and Mims, David and Holzapfel, Marco and Lukzen, Nikita N. and Steiner, Ulrich and Lambert, Christoph},
  note={Article Number: 054306}
}
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    <dcterms:abstract xml:lang="eng">A series of triads consisting of a triarylamine donor, a naphthalenediimide acceptor, and a palladium photosensitizer bridge was investigated for the photoinduced electron transfer processes and the spin chemistry involved. In this series, the ligand in the palladium photosensitizer was varied from bis-dipyrrinato to porphodimethenato and to a porphyrin. With the porphyrin photosensitizer, no charge separated state could be reached. This is caused by the direct relaxation of the excited photosensitizer to the ground state by intersystem crossing. The bis-dipyrrinato-palladium photosensitizer gave only a little yield (7%) of the charge separated state, which is due to the population of a metal centered triplet state and a concomitant geometrical rearrangement to a disphenoidal coordination sphere. This state relaxes rapidly to the ground state. In contrast, in the porphodimethenato-palladium triads, a long lived (μs to ms) charge separated state could be generated in high quantum yields (66%–74%) because, here, the population of a triplet metal centered state is inhibited by geometrical constraints. The magnetic field dependent transient absorption measurement of one of the porphodimethenato triads revealed a giant magnetic field effect by a factor of 26 on the signal amplitude of the charge separated state. This is the consequence of a magnetic field dependent triplet–singlet interconversion that inhibits the fast decay of the charge separated triplet state through the singlet recombination channel. A systematic comparative analysis of the spin-dependent kinetics in terms of three classical and one fully quantum theoretical methods is provided, shedding light on the pros and cons of each of them.</dcterms:abstract>
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