Manipulating photogenerated radical ion pair lifetimes in wirelike molecules using microwave pulses: Molecular spintronic gates

Tomoaki Miura, Michael R Wasielewski

Research output: Contribution to journalArticle

34 Citations (Scopus)

Abstract

We have studied spin-dependent charge transfer dynamics in wirelike donor-bridge-acceptor (D-B-A) molecules comprising a phenothiazine (PTZ) donor, an oligo(2,7-fluorene) (FLn) bridge, and a perylene-3,4:9,10- bis(dicarboximide) (PDI) acceptor, PTZ-FL3-PDI (1) and PTZ-FL 4-PDI (2), dissolved in the magnetic field-aligned nematic phase of 4-cyano-4′-n-pentylbiphenyl (5CB) at 295 K. Time-resolved EPR spectroscopy using both continuous wave and pulsed microwaves shows that the photogenerated radical pairs (RPs), PTZ+•-FL3-PDI-• and PTZ+•-FL4-PDI-•, recombine much faster from the singlet RP manifold than the triplet RP manifold. When a strong resonant microwave π pulse is applied following RP photogeneration in 1 and 2, the RP lifetimes increase about 50-fold as indicated by electron spin-echo detection. This result shows that the RP lifetime can be greatly extended by rapidly switching off fast triplet RP recombination.

Original languageEnglish
Pages (from-to)2844-2847
Number of pages4
JournalJournal of the American Chemical Society
Volume133
Issue number9
DOIs
Publication statusPublished - Mar 9 2011

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Magnetoelectronics
Microwaves
Ions
Molecules
Paramagnetic resonance
Charge transfer
Spectroscopy
Magnetic fields
Perylene
Electrons
Magnetic Fields
Genetic Recombination
Spectrum Analysis
phenothiazine

ASJC Scopus subject areas

  • Chemistry(all)
  • Catalysis
  • Biochemistry
  • Colloid and Surface Chemistry

Cite this

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title = "Manipulating photogenerated radical ion pair lifetimes in wirelike molecules using microwave pulses: Molecular spintronic gates",
abstract = "We have studied spin-dependent charge transfer dynamics in wirelike donor-bridge-acceptor (D-B-A) molecules comprising a phenothiazine (PTZ) donor, an oligo(2,7-fluorene) (FLn) bridge, and a perylene-3,4:9,10- bis(dicarboximide) (PDI) acceptor, PTZ-FL3-PDI (1) and PTZ-FL 4-PDI (2), dissolved in the magnetic field-aligned nematic phase of 4-cyano-4′-n-pentylbiphenyl (5CB) at 295 K. Time-resolved EPR spectroscopy using both continuous wave and pulsed microwaves shows that the photogenerated radical pairs (RPs), PTZ+•-FL3-PDI-• and PTZ+•-FL4-PDI-•, recombine much faster from the singlet RP manifold than the triplet RP manifold. When a strong resonant microwave π pulse is applied following RP photogeneration in 1 and 2, the RP lifetimes increase about 50-fold as indicated by electron spin-echo detection. This result shows that the RP lifetime can be greatly extended by rapidly switching off fast triplet RP recombination.",
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AB - We have studied spin-dependent charge transfer dynamics in wirelike donor-bridge-acceptor (D-B-A) molecules comprising a phenothiazine (PTZ) donor, an oligo(2,7-fluorene) (FLn) bridge, and a perylene-3,4:9,10- bis(dicarboximide) (PDI) acceptor, PTZ-FL3-PDI (1) and PTZ-FL 4-PDI (2), dissolved in the magnetic field-aligned nematic phase of 4-cyano-4′-n-pentylbiphenyl (5CB) at 295 K. Time-resolved EPR spectroscopy using both continuous wave and pulsed microwaves shows that the photogenerated radical pairs (RPs), PTZ+•-FL3-PDI-• and PTZ+•-FL4-PDI-•, recombine much faster from the singlet RP manifold than the triplet RP manifold. When a strong resonant microwave π pulse is applied following RP photogeneration in 1 and 2, the RP lifetimes increase about 50-fold as indicated by electron spin-echo detection. This result shows that the RP lifetime can be greatly extended by rapidly switching off fast triplet RP recombination.

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