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

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

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50 Scopus citations

Abstract

Employment of thin perovskite shells and metal halides as surface-passivants for colloidal quantum dots (CQDs) have been important, recent developments in CQD optoelectronics. These have opened the route to single-step deposited high-performing CQD solar cells. These promising architectures employ a QD 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 QD 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 photo-generated electrons, leading to enhanced photocurrent and fill factor compared to 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 - Aug 8 2017

Bibliographical note

KAUST Repository Item: Exported on 2020-10-01
Acknowledgements: 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.A., J. Z. F., G. W., S. H., and E. H. S. thank the 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.A. acknowledges financial support from the Connaught Fund.

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10.1021/acsenergylett.7b00540

https://repository.kaust.edu.sa/bitstream/10754/625298/1/acsenergylett.7b00540.pdf

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Kirmani, A. R., Garcia 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

@article{b5a4e4a08abe42dc854cdfdf3d57a75e,

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) have been important, recent developments in CQD optoelectronics. These have opened the route to single-step deposited high-performing CQD solar cells. These promising architectures employ a QD 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 QD 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 photo-generated electrons, leading to enhanced photocurrent and fill factor compared to 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 {Garcia de Arquer}, {F. Pelayo} and Fan, {James Z.} and Khan, {Jafar Iqbal} 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",

note = "KAUST Repository Item: Exported on 2020-10-01 Acknowledgements: 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.A., J. Z. F., G. W., S. H., and E. H. S. thank the 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.A. acknowledges financial support from the Connaught Fund.",

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doi = "10.1021/acsenergylett.7b00540",

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Kirmani, AR, Garcia 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

TY - JOUR

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

AU - Kirmani, Ahmad R.

AU - Garcia de Arquer, F. Pelayo

AU - Fan, James Z.

AU - Khan, Jafar Iqbal

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

N1 - KAUST Repository Item: Exported on 2020-10-01 Acknowledgements: 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.A., J. Z. F., G. W., S. H., and E. H. S. thank the 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.A. acknowledges financial support from the Connaught Fund.

PY - 2017/8/8

Y1 - 2017/8/8

N2 - Employment of thin perovskite shells and metal halides as surface-passivants for colloidal quantum dots (CQDs) have been important, recent developments in CQD optoelectronics. These have opened the route to single-step deposited high-performing CQD solar cells. These promising architectures employ a QD 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 QD 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 photo-generated electrons, leading to enhanced photocurrent and fill factor compared to 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) have been important, recent developments in CQD optoelectronics. These have opened the route to single-step deposited high-performing CQD solar cells. These promising architectures employ a QD 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 QD 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 photo-generated electrons, leading to enhanced photocurrent and fill factor compared to 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.

UR - http://hdl.handle.net/10754/625298

UR - http://pubs.acs.org/doi/abs/10.1021/acsenergylett.7b00540

UR - http://www.scopus.com/inward/record.url?scp=85033714531&partnerID=8YFLogxK

U2 - 10.1021/acsenergylett.7b00540

DO - 10.1021/acsenergylett.7b00540

M3 - Article

SN - 2380-8195

VL - 2

SP - 1952

EP - 1959

JO - ACS Energy Letters

JF - ACS Energy Letters

IS - 9

ER -

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

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