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

Abstract

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.

Authors:
; ; ; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Excitonics (CE)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1386746
DOE Contract Number:  
SC0001088
Resource Type:
Journal Article
Journal Name:
Nature Materials
Additional Journal Information:
Journal Volume: 13; Journal Issue: 11; Related Information: CE partners with Massachusetts Institute of Technology (lead); Brookhaven National Laboratory; Harvard University; Journal ID: ISSN 1476-1122
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; solar (photovoltaic), solid state lighting, photosynthesis (natural and artificial), charge transport, optics, synthesis (novel materials), synthesis (self-assembly), synthesis (scalable processing)

Citation Formats

Thompson, Nicholas J., Wilson, Mark W. B., Congreve, Daniel N., Brown, Patrick R., Scherer, Jennifer M., Bischof, Thomas S., Wu, Mengfei, Geva, Nadav, Welborn, Matthew, Voorhis, Troy Van, Bulović, Vladimir, Bawendi, Moungi G., and Baldo, Marc A. Energy harvesting of non-emissive triplet excitons in tetracene by emissive PbS nanocrystals. United States: N. p., 2014. Web. doi:10.1038/nmat4097.
Thompson, Nicholas J., Wilson, Mark W. B., Congreve, Daniel N., Brown, Patrick R., Scherer, Jennifer M., Bischof, Thomas S., Wu, Mengfei, Geva, Nadav, Welborn, Matthew, Voorhis, Troy Van, Bulović, Vladimir, Bawendi, Moungi G., & Baldo, Marc A. Energy harvesting of non-emissive triplet excitons in tetracene by emissive PbS nanocrystals. United States. doi:10.1038/nmat4097.
Thompson, Nicholas J., Wilson, Mark W. B., Congreve, Daniel N., Brown, Patrick R., Scherer, Jennifer M., Bischof, Thomas S., Wu, Mengfei, Geva, Nadav, Welborn, Matthew, Voorhis, Troy Van, Bulović, Vladimir, Bawendi, Moungi G., and Baldo, Marc A. Sun . "Energy harvesting of non-emissive triplet excitons in tetracene by emissive PbS nanocrystals". United States. doi:10.1038/nmat4097.
@article{osti_1386746,
title = {Energy harvesting of non-emissive triplet excitons in tetracene by emissive PbS nanocrystals},
author = {Thompson, Nicholas J. and Wilson, Mark W. B. and Congreve, Daniel N. and Brown, Patrick R. and Scherer, Jennifer M. and Bischof, Thomas S. and Wu, Mengfei and Geva, Nadav and Welborn, Matthew and Voorhis, Troy Van and Bulović, Vladimir and Bawendi, Moungi G. and Baldo, Marc A.},
abstractNote = {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.},
doi = {10.1038/nmat4097},
journal = {Nature Materials},
issn = {1476-1122},
number = 11,
volume = 13,
place = {United States},
year = {2014},
month = {10}
}

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