Molecular Doping of the Hole-Transporting Layer for Efficient, Single-Step-Deposited Colloidal Quantum Dot Photovoltaics

Ahmad R. Kirmani; F. Pelayo García De Arquer; James Z. Fan; Jafar I. Khan; Grant Walters; Sjoerd Hoogland; Nimer Wehbe; Marcel M. Said; Stephen Barlow; Frédéric Laquai; Seth R. Marder; Edward H. Sargent; Aram Amassian

doi:10.1021/acsenergylett.7b00540

Molecular Doping of the Hole-Transporting Layer for Efficient, Single-Step-Deposited Colloidal Quantum Dot Photovoltaics

Ahmad R. Kirmani, F. Pelayo García De Arquer, James Z. Fan, Jafar I. Khan, Grant Walters, Sjoerd Hoogland, Nimer Wehbe, Marcel M. Said, Stephen Barlow, Frédéric Laquai, Seth R. Marder, Edward H. Sargent, Aram Amassian^*

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

50 Scopus citations

Abstract

Employment of thin perovskite shells and metal halides as surface-passivants for colloidal quantum dots (CQDs) has been an important, recent development in CQD optoelectronics. These have opened the route to single-step-deposited high-performing CQD solar cells. These promising architectures employ a CQD hole-transporting layer (HTL) whose intrinsically shallow Fermi level (E_F) restricts band-bending at maximum power-point during solar cell operation limiting charge collection. Here, we demonstrate a generalized approach to effectively balance band-edge energy levels of the main CQD absorber and charge-transport layer for these high-performance solar cells. Briefly soaking the CQD HTL in a solution of the metal-organic p-dopant, molybdenum tris(1-(trifluoroacetyl)-2-(trifluoromethyl)ethane-1,2-dithiolene), effectively deepens its Fermi level, resulting in enhanced band bending at the HTL:absorber junction. This blocks the back-flow of photogenerated electrons, leading to enhanced photocurrent and fill factor compared to those of undoped devices. We demonstrate 9.0% perovskite-shelled and 9.5% metal-halide-passivated CQD solar cells, both achieving ca. 10% relative enhancements over undoped baselines.

Original language	English (US)
Pages (from-to)	1952-1959
Number of pages	8
Journal	ACS Energy Letters
Volume	2
Issue number	9
DOIs	https://doi.org/10.1021/acsenergylett.7b00540
State	Published - Sep 8 2017

Funding

The authors thank Yadong Zhang (Georgia Institute of Technology) for the chemical synthesis of the metal−organic complex, Mo(tfd-COCF3)3, used in this study. F.P.G.d.A., J.Z.F., G.W., S.H., and E.H.S. acknowledge Award KUS-11-009-21 from King Abdullah University of Science and Technology (KAUST), the Ontario Research Fund − Research Excellence Program, and the Natural Sciences and Engineering Research Council of Canada (NSERC). M.M.S., S.B., and S.R.M. thank the Office of Naval Research for support through N00014-14-1-0126. F.P.G.d.A. acknowledges financial support from the Connaught Fund.

ASJC Scopus subject areas

Chemistry (miscellaneous)
Renewable Energy, Sustainability and the Environment
Fuel Technology
Energy Engineering and Power Technology
Materials Chemistry

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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Kirmani, A. R., García De Arquer, F. P., Fan, J. Z., Khan, J. I., Walters, G., Hoogland, S., Wehbe, N., Said, M. M., Barlow, S., Laquai, F., Marder, S. R., Sargent, E. H., & Amassian, A. (2017). Molecular Doping of the Hole-Transporting Layer for Efficient, Single-Step-Deposited Colloidal Quantum Dot Photovoltaics. ACS Energy Letters, 2(9), 1952-1959. https://doi.org/10.1021/acsenergylett.7b00540

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title = "Molecular Doping of the Hole-Transporting Layer for Efficient, Single-Step-Deposited Colloidal Quantum Dot Photovoltaics",

abstract = "Employment of thin perovskite shells and metal halides as surface-passivants for colloidal quantum dots (CQDs) has been an important, recent development in CQD optoelectronics. These have opened the route to single-step-deposited high-performing CQD solar cells. These promising architectures employ a CQD hole-transporting layer (HTL) whose intrinsically shallow Fermi level (EF) restricts band-bending at maximum power-point during solar cell operation limiting charge collection. Here, we demonstrate a generalized approach to effectively balance band-edge energy levels of the main CQD absorber and charge-transport layer for these high-performance solar cells. Briefly soaking the CQD HTL in a solution of the metal-organic p-dopant, molybdenum tris(1-(trifluoroacetyl)-2-(trifluoromethyl)ethane-1,2-dithiolene), effectively deepens its Fermi level, resulting in enhanced band bending at the HTL:absorber junction. This blocks the back-flow of photogenerated electrons, leading to enhanced photocurrent and fill factor compared to those of undoped devices. We demonstrate 9.0% perovskite-shelled and 9.5% metal-halide-passivated CQD solar cells, both achieving ca. 10% relative enhancements over undoped baselines.",

author = "Kirmani, {Ahmad R.} and {Garc{\'i}a De Arquer}, {F. Pelayo} and Fan, {James Z.} and Khan, {Jafar I.} and Grant Walters and Sjoerd Hoogland and Nimer Wehbe and Said, {Marcel M.} and Stephen Barlow and Fr{\'e}d{\'e}ric Laquai and Marder, {Seth R.} and Sargent, {Edward H.} and Aram Amassian",

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Kirmani, AR, García De Arquer, FP, Fan, JZ, Khan, JI, Walters, G, Hoogland, S, Wehbe, N, Said, MM, Barlow, S, Laquai, F, Marder, SR, Sargent, EH & Amassian, A 2017, 'Molecular Doping of the Hole-Transporting Layer for Efficient, Single-Step-Deposited Colloidal Quantum Dot Photovoltaics', ACS Energy Letters, vol. 2, no. 9, pp. 1952-1959. https://doi.org/10.1021/acsenergylett.7b00540

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T1 - Molecular Doping of the Hole-Transporting Layer for Efficient, Single-Step-Deposited Colloidal Quantum Dot Photovoltaics

AU - Kirmani, Ahmad R.

AU - García De Arquer, F. Pelayo

AU - Fan, James Z.

AU - Khan, Jafar I.

AU - Walters, Grant

AU - Hoogland, Sjoerd

AU - Wehbe, Nimer

AU - Said, Marcel M.

AU - Barlow, Stephen

AU - Laquai, Frédéric

AU - Marder, Seth R.

AU - Sargent, Edward H.

AU - Amassian, Aram

PY - 2017/9/8

Y1 - 2017/9/8

N2 - Employment of thin perovskite shells and metal halides as surface-passivants for colloidal quantum dots (CQDs) has been an important, recent development in CQD optoelectronics. These have opened the route to single-step-deposited high-performing CQD solar cells. These promising architectures employ a CQD hole-transporting layer (HTL) whose intrinsically shallow Fermi level (EF) restricts band-bending at maximum power-point during solar cell operation limiting charge collection. Here, we demonstrate a generalized approach to effectively balance band-edge energy levels of the main CQD absorber and charge-transport layer for these high-performance solar cells. Briefly soaking the CQD HTL in a solution of the metal-organic p-dopant, molybdenum tris(1-(trifluoroacetyl)-2-(trifluoromethyl)ethane-1,2-dithiolene), effectively deepens its Fermi level, resulting in enhanced band bending at the HTL:absorber junction. This blocks the back-flow of photogenerated electrons, leading to enhanced photocurrent and fill factor compared to those of undoped devices. We demonstrate 9.0% perovskite-shelled and 9.5% metal-halide-passivated CQD solar cells, both achieving ca. 10% relative enhancements over undoped baselines.

AB - Employment of thin perovskite shells and metal halides as surface-passivants for colloidal quantum dots (CQDs) has been an important, recent development in CQD optoelectronics. These have opened the route to single-step-deposited high-performing CQD solar cells. These promising architectures employ a CQD hole-transporting layer (HTL) whose intrinsically shallow Fermi level (EF) restricts band-bending at maximum power-point during solar cell operation limiting charge collection. Here, we demonstrate a generalized approach to effectively balance band-edge energy levels of the main CQD absorber and charge-transport layer for these high-performance solar cells. Briefly soaking the CQD HTL in a solution of the metal-organic p-dopant, molybdenum tris(1-(trifluoroacetyl)-2-(trifluoromethyl)ethane-1,2-dithiolene), effectively deepens its Fermi level, resulting in enhanced band bending at the HTL:absorber junction. This blocks the back-flow of photogenerated electrons, leading to enhanced photocurrent and fill factor compared to those of undoped devices. We demonstrate 9.0% perovskite-shelled and 9.5% metal-halide-passivated CQD solar cells, both achieving ca. 10% relative enhancements over undoped baselines.

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JF - ACS Energy Letters

IS - 9

ER -

Molecular Doping of the Hole-Transporting Layer for Efficient, Single-Step-Deposited Colloidal Quantum Dot Photovoltaics

Abstract

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ASJC Scopus subject areas

UN SDGs

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