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Title: Sensitization of silicon by singlet exciton fission in tetracene

Abstract

Silicon dominates contemporary solar cell technologies. Yet when absorbing photons, silicon (like other semiconductors) wastes energy in excess of its bandgap. Reducing these thermalization losses and enabling better sensitivity to light is possible by sensitizing the silicon solar cell using singlet exciton fission, in which two excited states with triplet spin character (triplet excitons) are generated from a photoexcited state of higher energy with singlet spin character (a singlet exciton). Singlet exciton fission in the molecular semiconductor tetracene is known to generate triplet excitons that are energetically matched to the silicon bandgap. When the triplet excitons are transferred to silicon they create additional electron–hole pairs, promising to increase cell efficiencies from the single-junction limit of 29 per cent to as high as 35 per cent. In this report we reduce the thickness of the protective hafnium oxynitride layer at the surface of a silicon solar cell to just eight angstroms, using electric-field-effect passivation to enable the efficient energy transfer of the triplet excitons formed in the tetracene. The maximum combined yield of the fission in tetracene and the energy transfer to silicon is around 133 per cent, establishing the potential of singlet exciton fission to increase the efficiencies of siliconmore » solar cells and reduce the cost of the energy that they generate.« less

Authors:
 [1];  [1];  [1];  [2];  [1];  [1];  [1];  [3];  [2];  [1];  [1]
  1. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  2. Princeton Univ., NJ (United States)
  3. Harvard Univ., Cambridge, MA (United States); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Excitonics (CE); Princeton Univ., NJ (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; National Science Foundation (NSF)
OSTI Identifier:
1595459
Grant/Contract Number:  
SC0012458; SC0001088; DGE-1656466
Resource Type:
Accepted Manuscript
Journal Name:
Nature (London)
Additional Journal Information:
Journal Name: Nature (London); Journal Volume: 571; Journal Issue: 7763; Journal ID: ISSN 0028-0836
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
42 ENGINEERING

Citation Formats

Einzinger, Markus, Wu, Tony, Kompalla, Julia F., Smith, Hannah L., Perkinson, Collin F., Nienhaus, Lea, Wieghold, Sarah, Congreve, Daniel N., Kahn, Antoine, Bawendi, Moungi G., and Baldo, Marc A. Sensitization of silicon by singlet exciton fission in tetracene. United States: N. p., 2019. Web. doi:10.1038/s41586-019-1339-4.
Einzinger, Markus, Wu, Tony, Kompalla, Julia F., Smith, Hannah L., Perkinson, Collin F., Nienhaus, Lea, Wieghold, Sarah, Congreve, Daniel N., Kahn, Antoine, Bawendi, Moungi G., & Baldo, Marc A. Sensitization of silicon by singlet exciton fission in tetracene. United States. doi:https://doi.org/10.1038/s41586-019-1339-4
Einzinger, Markus, Wu, Tony, Kompalla, Julia F., Smith, Hannah L., Perkinson, Collin F., Nienhaus, Lea, Wieghold, Sarah, Congreve, Daniel N., Kahn, Antoine, Bawendi, Moungi G., and Baldo, Marc A. Wed . "Sensitization of silicon by singlet exciton fission in tetracene". United States. doi:https://doi.org/10.1038/s41586-019-1339-4. https://www.osti.gov/servlets/purl/1595459.
@article{osti_1595459,
title = {Sensitization of silicon by singlet exciton fission in tetracene},
author = {Einzinger, Markus and Wu, Tony and Kompalla, Julia F. and Smith, Hannah L. and Perkinson, Collin F. and Nienhaus, Lea and Wieghold, Sarah and Congreve, Daniel N. and Kahn, Antoine and Bawendi, Moungi G. and Baldo, Marc A.},
abstractNote = {Silicon dominates contemporary solar cell technologies. Yet when absorbing photons, silicon (like other semiconductors) wastes energy in excess of its bandgap. Reducing these thermalization losses and enabling better sensitivity to light is possible by sensitizing the silicon solar cell using singlet exciton fission, in which two excited states with triplet spin character (triplet excitons) are generated from a photoexcited state of higher energy with singlet spin character (a singlet exciton). Singlet exciton fission in the molecular semiconductor tetracene is known to generate triplet excitons that are energetically matched to the silicon bandgap. When the triplet excitons are transferred to silicon they create additional electron–hole pairs, promising to increase cell efficiencies from the single-junction limit of 29 per cent to as high as 35 per cent. In this report we reduce the thickness of the protective hafnium oxynitride layer at the surface of a silicon solar cell to just eight angstroms, using electric-field-effect passivation to enable the efficient energy transfer of the triplet excitons formed in the tetracene. The maximum combined yield of the fission in tetracene and the energy transfer to silicon is around 133 per cent, establishing the potential of singlet exciton fission to increase the efficiencies of silicon solar cells and reduce the cost of the energy that they generate.},
doi = {10.1038/s41586-019-1339-4},
journal = {Nature (London)},
number = 7763,
volume = 571,
place = {United States},
year = {2019},
month = {7}
}

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Works referenced in this record:

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    Works referencing / citing this record:

    Surface passivation of crystalline silicon solar cells: a review
    journal, January 2000


    Simple Patterning via Adhesion between a Buffered-Oxide Etchant-Treated PDMS Stamp and a SiO 2 Substrate
    journal, July 2007

    • Kim, Y. -K.; Kim, G. T.; Ha, J. S.
    • Advanced Functional Materials, Vol. 17, Issue 13
    • DOI: 10.1002/adfm.200700217

    Dielectric surface passivation for silicon solar cells: A review
    journal, June 2017

    • Bonilla, Ruy S.; Hoex, Bram; Hamer, Phillip
    • physica status solidi (a), Vol. 214, Issue 7
    • DOI: 10.1002/pssa.201700293

    Characterization of Polydimethylsiloxane (PDMS) Properties for Biomedical Micro/Nanosystems
    journal, December 2005


    Bimolecular radiationless transitions in crystalline tetracene
    journal, September 1968


    Fission of singlet excitons into pairs of triplet excitons in tetracene crystals
    journal, June 1969


    Quenching of molecular fluorescence near the surface of a semiconductor
    journal, February 1983


    Dynamics of molecular excitons near a semiconductor surface studied by fluorescence quenching of polycrystalline tetracene on silicon
    journal, May 2014


    Electron-hole interaction energy in the organic molecular semiconductor PTCDA
    journal, June 1997


    Dopant-Free All-Back-Contact Si Nanohole Solar Cells Using MoO x and LiF Films
    journal, January 2016


    Atomic Layer Deposition of Insulating Hafnium and Zirconium Nitrides
    journal, September 2004

    • Becker, Jill S.; Kim, Esther; Gordon, Roy G.
    • Chemistry of Materials, Vol. 16, Issue 18
    • DOI: 10.1021/cm049516y

    Singlet Fission
    journal, November 2010

    • Smith, Millicent B.; Michl, Josef
    • Chemical Reviews, Vol. 110, Issue 11
    • DOI: 10.1021/cr1002613

    Harnessing singlet exciton fission to break the Shockley–Queisser limit
    journal, October 2017


    A transferable model for singlet-fission kinetics
    journal, May 2014

    • Yost, Shane R.; Lee, Jiye; Wilson, Mark W. B.
    • Nature Chemistry, Vol. 6, Issue 6
    • DOI: 10.1038/nchem.1945

    Commercial progress and challenges for photovoltaics
    journal, January 2016


    Resonant energy transfer of triplet excitons from pentacene to PbSe nanocrystals
    journal, October 2014

    • Tabachnyk, Maxim; Ehrler, Bruno; Gélinas, Simon
    • Nature Materials, Vol. 13, Issue 11
    • DOI: 10.1038/nmat4093

    Energy harvesting of non-emissive triplet excitons in tetracene by emissive PbS nanocrystals
    journal, October 2014

    • Thompson, Nicholas J.; Wilson, Mark W. B.; Congreve, Daniel N.
    • Nature Materials, Vol. 13, Issue 11
    • DOI: 10.1038/nmat4097

    Crystalline silicon solar cells with tetracene interlayers: the path to silicon-singlet fission heterojunction devices
    journal, January 2018

    • MacQueen, Rowan W.; Liebhaber, Martin; Niederhausen, Jens
    • Materials Horizons, Vol. 5, Issue 6
    • DOI: 10.1039/c8mh00853a

    A Theory of Sensitized Luminescence in Solids
    journal, May 1953

    • Dexter, D. L.
    • The Journal of Chemical Physics, Vol. 21, Issue 5, p. 836-850
    • DOI: 10.1063/1.1699044

    Detailed Balance Limit of Efficiency of p‐n Junction Solar Cells
    journal, March 1961

    • Shockley, William; Queisser, Hans J.
    • Journal of Applied Physics, Vol. 32, Issue 3, p. 510-519
    • DOI: 10.1063/1.1736034

    Solar conversion efficiency of photovoltaic and photoelectrolysis cells with carrier multiplication absorbers
    journal, October 2006

    • Hanna, M. C.; Nozik, A. J.
    • Journal of Applied Physics, Vol. 100, Issue 7
    • DOI: 10.1063/1.2356795

    Singlet fission efficiency in tetracene-based organic solar cells
    journal, May 2014

    • Wu, Tony C.; Thompson, Nicholas J.; Congreve, Daniel N.
    • Applied Physics Letters, Vol. 104, Issue 19
    • DOI: 10.1063/1.4876600

    Kinematics of Exciton-Exciton Annihilation in Molecular Crystals
    journal, February 1970


    Effect of Magnetic Field on the Fluorescence of Tetracene Crystals: Exciton Fission
    journal, March 1969


    External Quantum Efficiency Above 100% in a Singlet-Exciton-Fission-Based Organic Photovoltaic Cell
    journal, April 2013


    Recent Advances in Singlet Fission
    journal, April 2013


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