4.8 Article

Energy harvesting of non-emissive triplet excitons in tetracene by emissive PbS nanocrystals

Journal

NATURE MATERIALS
Volume 13, Issue 11, Pages 1039-1043

Publisher

NATURE PUBLISHING GROUP
DOI: 10.1038/NMAT4097

Keywords

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Funding

  1. Center for Excitonics, an Energy Frontier Research Center - US Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001088]
  2. National Science Foundation Graduate Research Fellowship [1122374]
  3. Department of Defense, Air Force Office of Scientific Research, National Defense Science and Engineering Graduate (NDSEG) Fellowship [FA9550-11-C-0028, 32 CFR 168a]
  4. US Army through the Institute for Soldier Nanotechnology [W911NF-13-D-0001]

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Triplet excitons are ubiquitous in organic optoelectronics, but they are often an undesirable energy sink because they are spin-forbidden from emitting light and their high binding energy hinders the generation of free electron-hole pairs. Harvesting their energy is consequently an important technological challenge. Here, we demonstrate direct excitonic energy transfer from 'dark' triplets in the organic semiconductor tetracene to colloidal PbS nanocrystals, thereby successfully harnessing molecular triplet excitons in the near infrared. Steady-state excitation spectra, supported by transient photoluminescence studies, demonstrate that the transfer efficiency is at least (90 +/- 13)%. The mechanism is a Dexter hopping process consisting of the simultaneous exchange of two electrons. Triplet exciton transfer to nanocrystals is expected to be broadly applicable in solar and near-infrared light-emitting applications, where effective molecular phosphors are lacking at present. In particular, this route to 'brighten' low-energy molecular triplet excitons may permit singlet exciton fission sensitization of conventional silicon solar cells.

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