Charge transport in photofunctional nanoparticles self-assembled from zinc 5,10,15,20-tetrakis(perylenediimide)porphyrin building blocks

Tamar Van der Boom, Ryan T. Hayes, Yongyu Zhao, Patrick J. Bushard, Emily A Weiss, Michael R Wasielewski

Research output: Contribution to journalArticle

337 Citations (Scopus)

Abstract

Molecules designed to carry out photochemical energy conversion typically employ several sequential electron transfers, as do photosynthetic proteins. Yet, these molecules typically do not achieve the extensive charge transport characteristic of semiconductor devices. We have prepared a large molecule in which four perylene-3,4:9,10-tetracarboxydiimide (PDI) molecules that both collect photons and accept electrons are attached to a central zinc 5,10,15,20-tetraphenylporphyrin (ZnTPP) electron donor. This molecule self-assembles into ordered nanoparticles both in solution and in the solid-state, driven by van der Waals stacking of the PDI molecules. Photoexcitation of the nanoparticles results in quantitative charge separation in 3.2 ps to form ZnTPP+PDI- radical ion pairs, in which the radical anion rapidly migrates to PDI molecules that are, on average, 21 Å away, as evidenced by magnetic field effects on the yield of the PDI triplet state that results from radical ion pair recombination. These nanoparticles exhibit charge transport properties that combine important features from both photosynthetic and semiconductor photoconversion systems.

Original languageEnglish
Pages (from-to)9582-9590
Number of pages9
JournalJournal of the American Chemical Society
Volume124
Issue number32
DOIs
Publication statusPublished - Aug 14 2002

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Porphyrins
Nanoparticles
Charge transfer
Zinc
Semiconductors
Electrons
Molecules
Perylene
Ions
Magnetic Fields
Photons
Genetic Recombination
Anions
Equipment and Supplies
Magnetic field effects
Photoexcitation
Semiconductor devices
perylenediimide
Energy conversion
Proteins

ASJC Scopus subject areas

  • Chemistry(all)

Cite this

Charge transport in photofunctional nanoparticles self-assembled from zinc 5,10,15,20-tetrakis(perylenediimide)porphyrin building blocks. / Van der Boom, Tamar; Hayes, Ryan T.; Zhao, Yongyu; Bushard, Patrick J.; Weiss, Emily A; Wasielewski, Michael R.

In: Journal of the American Chemical Society, Vol. 124, No. 32, 14.08.2002, p. 9582-9590.

Research output: Contribution to journalArticle

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abstract = "Molecules designed to carry out photochemical energy conversion typically employ several sequential electron transfers, as do photosynthetic proteins. Yet, these molecules typically do not achieve the extensive charge transport characteristic of semiconductor devices. We have prepared a large molecule in which four perylene-3,4:9,10-tetracarboxydiimide (PDI) molecules that both collect photons and accept electrons are attached to a central zinc 5,10,15,20-tetraphenylporphyrin (ZnTPP) electron donor. This molecule self-assembles into ordered nanoparticles both in solution and in the solid-state, driven by van der Waals stacking of the PDI molecules. Photoexcitation of the nanoparticles results in quantitative charge separation in 3.2 ps to form ZnTPP+PDI- radical ion pairs, in which the radical anion rapidly migrates to PDI molecules that are, on average, 21 {\AA} away, as evidenced by magnetic field effects on the yield of the PDI triplet state that results from radical ion pair recombination. These nanoparticles exhibit charge transport properties that combine important features from both photosynthetic and semiconductor photoconversion systems.",
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