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

Journal Article · · Nature Materials
DOI:https://doi.org/10.1038/nmat4097· OSTI ID:1386746

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.

Research Organization:
Energy Frontier Research Centers (EFRC) (United States). Center for Excitonics (CE)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
DOE Contract Number:
SC0001088
OSTI ID:
1386746
Journal Information:
Nature Materials, Vol. 13, Issue 11; Related Information: CE partners with Massachusetts Institute of Technology (lead); Brookhaven National Laboratory; Harvard University; ISSN 1476-1122
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English

References (34)

Quantum dots in a magnetic field: Role of electron-electron interactions journal July 1990
The Structure and Dynamics of Molecular Excitons journal April 2014
Slow light enhanced singlet exciton fission solar cells with a 126% yield of electrons per photon journal December 2013
The role of spin in the kinetic control of recombination in organic photovoltaics journal August 2013
Excitonic singlet-triplet ratio in a semiconducting organic thin film journal November 1999
Recent Advances in Singlet Fission journal April 2013
What controls triplet exciton transfer in organic semiconductors? journal January 2011
Temperature-Independent Singlet Exciton Fission in Tetracene journal October 2013
External Quantum Efficiency Above 100% in a Singlet-Exciton-Fission-Based Organic Photovoltaic Cell journal April 2013
Excitonic singlet-triplet ratios in molecular and polymeric organic materials journal August 2003
Absolute Photoluminescence Quantum Yields of IR-26 Dye, PbS, and PbSe Quantum Dots journal July 2010
Photoluminescence of CdSe/ZnS core/shell quantum dots enhanced by energy transfer from a phosphorescent donor journal June 2006
Fission of singlet excitons into pairs of triplet excitons in tetracene crystals journal June 1969
The Dynamics of Singlet Fission in Crystalline Tetracene and Covalent Analogs journal January 2013
Room temperature triplet state spectroscopy of organic semiconductors journal January 2014
Controlling Charge Separation and Recombination Rates in CdSe/ZnS Type I Core−Shell Quantum Dots by Shell Thicknesses journal October 2010
Dynamics of molecular excitons near a semiconductor surface studied by fluorescence quenching of polycrystalline tetracene on silicon journal May 2014
Size-Dependent Valence and Conduction Band-Edge Energies of Semiconductor Nanocrystals journal June 2011
Spectroscopic Approach to Energetics of Exciton Fission and Fusion in Tetracene Crystals journal May 1971
Size-Dependent Optical Properties of Colloidal PbS Quantum Dots journal September 2009
The exciton dynamics in tetracene thin films journal January 2013
A Theory of Sensitized Luminescence in Solids journal May 1953
p-Type PbSe and PbS Quantum Dot Solids Prepared with Short-Chain Acids and Diacids journal March 2010
Highly efficient phosphorescent emission from organic electroluminescent devices journal September 1998
Singlet Exciton Fission in Polycrystalline Pentacene: From Photophysics toward Devices journal May 2013
Singlet Exciton Fission Photovoltaics journal April 2013
Singlet fission efficiency in tetracene-based organic solar cells journal May 2014
The dependence of singlet exciton relaxation on excitation density and temperature in polycrystalline tetracene thin films: Kinetic evidence for a dark intermediate state and implications for singlet fission journal December 2011
Triplet Exciton Dissociation in Singlet Exciton Fission Photovoltaics journal September 2012
In situ measurement of exciton energy in hybrid singlet-fission solar cells journal January 2012
Distance Dependence of Electronic Energy Transfer to Semiconductor Surfaces: n 3 π * Pyrazine/GaAs(110) journal April 1983
Re-evaluating the Role of Sterics and Electronic Coupling in Determining the Open-Circuit Voltage of Organic Solar Cells journal July 2013
Quenching of molecular fluorescence near the surface of a semiconductor journal February 1983
A transferable model for singlet-fission kinetics journal May 2014