Discovery of blue singlet exciton fission molecules via a high-throughput virtual screening and experimental approach
Abstract
Singlet exciton fission is a mechanism that could potentially enable solar cells to surpass the Shockley-Queisser efficiency limit by converting single high-energy photons into two lower-energy triplet excitons with minimal thermalization loss. The ability to make use of singlet exciton fission to enhance solar cell efficiencies has been limited, however, by the sparsity of singlet fission materials with triplet energies above the bandgaps of common semiconductors such as Si and GaAs. Here, we employ a high-throughput virtual screening procedure to discover new organic singlet exciton fission candidate materials with high-energy (>1.4 eV) triplet excitons. After exploring a search space of 4482 molecules and screening them using time-dependent density functional theory, we identify 88 novel singlet exciton fission candidate materials based on anthracene derivatives. Subsequent purification and characterization of several of these candidates yield two new singlet exciton fission materials: 9,10-dicyanoanthracene (DCA) and 9,10-dichlorooctafluoroanthracene (DCOFA), with triplet energies of 1.54 eV and 1.51 eV, respectively. These materials are readily available and low-cost, making them interesting candidates for exothermic singlet exciton fission sensitization of solar cells. However, formation of triplet excitons in DCA and DCOFA is found to occur via hot singlet exciton fission with excitation energies above ~3.64 eV, and prominentmore »
- Authors:
-
- Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Chemistry
- Harvard Univ., Cambridge, MA (United States)
- Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Electrical Engineering and Computer Science
- Harvard Univ., Cambridge, MA (United States); Univ. of Toronto, ON (Canada)
- Publication Date:
- Research Org.:
- Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC)
- OSTI Identifier:
- 1609912
- Alternate Identifier(s):
- OSTI ID: 1576867
- Grant/Contract Number:
- FG02-07ER46454; FG02-07ER46474; SC0001088
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 151; Journal Issue: 12; Journal ID: ISSN 0021-9606
- Publisher:
- American Institute of Physics (AIP)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; Chemistry; Physics; Semiconductors; Solar cells; Time dependent density functional theory; Chemical properties; Photoluminescence; Excitons; Equilibrium thermodynamics; Excitation energies; Phosphorescence; Magnetic fields
Citation Formats
Perkinson, Collin F., Tabor, Daniel P., Einzinger, Markus, Sheberla, Dennis, Utzat, Hendrik, Lin, Ting-An, Congreve, Daniel N., Bawendi, Moungi G., Aspuru-Guzik, Alán, and Baldo, Marc A. Discovery of blue singlet exciton fission molecules via a high-throughput virtual screening and experimental approach. United States: N. p., 2019.
Web. doi:10.1063/1.5114789.
Perkinson, Collin F., Tabor, Daniel P., Einzinger, Markus, Sheberla, Dennis, Utzat, Hendrik, Lin, Ting-An, Congreve, Daniel N., Bawendi, Moungi G., Aspuru-Guzik, Alán, & Baldo, Marc A. Discovery of blue singlet exciton fission molecules via a high-throughput virtual screening and experimental approach. United States. https://doi.org/10.1063/1.5114789
Perkinson, Collin F., Tabor, Daniel P., Einzinger, Markus, Sheberla, Dennis, Utzat, Hendrik, Lin, Ting-An, Congreve, Daniel N., Bawendi, Moungi G., Aspuru-Guzik, Alán, and Baldo, Marc A. Tue .
"Discovery of blue singlet exciton fission molecules via a high-throughput virtual screening and experimental approach". United States. https://doi.org/10.1063/1.5114789. https://www.osti.gov/servlets/purl/1609912.
@article{osti_1609912,
title = {Discovery of blue singlet exciton fission molecules via a high-throughput virtual screening and experimental approach},
author = {Perkinson, Collin F. and Tabor, Daniel P. and Einzinger, Markus and Sheberla, Dennis and Utzat, Hendrik and Lin, Ting-An and Congreve, Daniel N. and Bawendi, Moungi G. and Aspuru-Guzik, Alán and Baldo, Marc A.},
abstractNote = {Singlet exciton fission is a mechanism that could potentially enable solar cells to surpass the Shockley-Queisser efficiency limit by converting single high-energy photons into two lower-energy triplet excitons with minimal thermalization loss. The ability to make use of singlet exciton fission to enhance solar cell efficiencies has been limited, however, by the sparsity of singlet fission materials with triplet energies above the bandgaps of common semiconductors such as Si and GaAs. Here, we employ a high-throughput virtual screening procedure to discover new organic singlet exciton fission candidate materials with high-energy (>1.4 eV) triplet excitons. After exploring a search space of 4482 molecules and screening them using time-dependent density functional theory, we identify 88 novel singlet exciton fission candidate materials based on anthracene derivatives. Subsequent purification and characterization of several of these candidates yield two new singlet exciton fission materials: 9,10-dicyanoanthracene (DCA) and 9,10-dichlorooctafluoroanthracene (DCOFA), with triplet energies of 1.54 eV and 1.51 eV, respectively. These materials are readily available and low-cost, making them interesting candidates for exothermic singlet exciton fission sensitization of solar cells. However, formation of triplet excitons in DCA and DCOFA is found to occur via hot singlet exciton fission with excitation energies above ~3.64 eV, and prominent excimer formation in the solid state will need to be overcome in order to make DCA and DCOFA viable candidates for use in a practical device.},
doi = {10.1063/1.5114789},
journal = {Journal of Chemical Physics},
number = 12,
volume = 151,
place = {United States},
year = {Tue Sep 24 00:00:00 EDT 2019},
month = {Tue Sep 24 00:00:00 EDT 2019}
}
Web of Science
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