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Research Article

Monolithic perovskite/silicon tandem solar cell with >29% efficiency by enhanced hole extraction

Amran Al-Ashouri https://orcid.org/0000-0001-5512-8034, Eike Köhnen https://orcid.org/0000-0002-3637-4907, Bor Li https://orcid.org/0000-0003-3895-0792, Artiom Magomedov https://orcid.org/0000-0003-3159-1870, Hannes Hempel https://orcid.org/0000-0001-9689-9644, Pietro Caprioglio https://orcid.org/0000-0002-3465-2475, José A. Márquez https://orcid.org/0000-0002-8173-2566, Anna Belen Morales Vilches https://orcid.org/0000-0001-8819-1312, Ernestas Kasparavicius, Joel A. Smith https://orcid.org/0000-0001-6889-4408, Nga Phung https://orcid.org/0000-0002-0328-6791, Dorothee Menzel https://orcid.org/0000-0002-6303-8909, Max Grischek https://orcid.org/0000-0002-9786-4854, Lukas Kegelmann https://orcid.org/0000-0001-8918-5096, Dieter Skroblin https://orcid.org/0000-0002-8197-2113, Christian Gollwitzer https://orcid.org/0000-0002-6437-8825, Tadas Malinauskas https://orcid.org/0000-0002-5478-6550, Marko Jošt https://orcid.org/0000-0003-2754-1467, Gašper Matič https://orcid.org/0000-0001-7024-1588, Bernd Rech https://orcid.org/0000-0002-9718-8665, Rutger Schlatmann https://orcid.org/0000-0002-5951-9435, Marko Topič https://orcid.org/0000-0001-8089-2974, Lars Korte https://orcid.org/0000-0002-9207-9048, Antonio Abate https://orcid.org/0000-0002-3012-3541, Bernd Stannowski https://orcid.org/0000-0003-0130-3954, Dieter Neher https://orcid.org/0000-0001-6618-8403, Martin Stolterfoht https://orcid.org/0000-0002-4023-2178, Thomas Unold https://orcid.org/0000-0002-5750-0693, Vytautas Getautis https://orcid.org/0000-0001-7695-4677, and Steve Albrecht https://orcid.org/0000-0001-9962-9535 [email protected]
Science • 11 Dec 2020 • Vol 370, Issue 6522 • pp. 1300-1309 • DOI: 10.1126/science.abd4016
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Efficiency from hole-selective contacts

Perovskite/silicon tandem solar cells must stabilize a perovskite material with a wide bandgap and also maintain efficient charge carrier transport. Al-Ashouri et al. stabilized a perovskite with a 1.68–electron volt bandgap with a self-assembled monolayer that acted as an efficient hole-selective contact that minimizes nonradiative carrier recombination. In air without encapsulation, a tandem silicon cell retained 95% of its initial power conversion efficiency of 29% after 300 hours of operation.
Science, this issue p. 1300

Abstract

Tandem solar cells that pair silicon with a metal halide perovskite are a promising option for surpassing the single-cell efficiency limit. We report a monolithic perovskite/silicon tandem with a certified power conversion efficiency of 29.15%. The perovskite absorber, with a bandgap of 1.68 electron volts, remained phase-stable under illumination through a combination of fast hole extraction and minimized nonradiative recombination at the hole-selective interface. These features were made possible by a self-assembled, methyl-substituted carbazole monolayer as the hole-selective layer in the perovskite cell. The accelerated hole extraction was linked to a low ideality factor of 1.26 and single-junction fill factors of up to 84%, while enabling a tandem open-circuit voltage of as high as 1.92 volts. In air, without encapsulation, a tandem retained 95% of its initial efficiency after 300 hours of operation.
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Supplementary Material

Summary

Materials and Methods
Supplementary Text
Figs. S1 to S39
Tables S1 to S3
References (70–85)

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Science
Volume 370 | Issue 6522
11 December 2020

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Copyright © 2020 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works.
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Received: 19 June 2020
Accepted: 30 October 2020
Published in print: 11 December 2020

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Acknowledgments

We thank M. Gabernig, C. Ferber, T. Lußky, H. Heinz, C. Klimm, and M. Muske at the Institute for Silicon Photovoltaics, Helmholtz-Zentrum Berlin (HZB), and T. Hänel, T. Henschel, M. Zelt, H. Rhein, K. Meyer-Stillrich, and M. Hartig at PVcomB (HZB) for technical assistance. A.A.-A. thanks A. Merdasa for his expertise during construction of the steady-state PL setup. Ei.K. and S.A. thank C. Wolff (University of Potsdam) and K. Brinkmann (University of Wuppertal) for fruitful discussion at the beginning of the project. A.M. acknowledges A. Drevilkauskaite for help with the synthesis of 4PACz and 6PACz materials. Funding: Supported by Federal Ministry for Education and Research (BMBF) grant 03SF0540 within the project “Materialforschung für die Energiewende”; the Federal Ministry for Economic Affairs and Energy (BMWi)–funded project ProTandem (0324288C); the HyPerCells graduate school; the Helmholtz Association within the HySPRINT Innovation lab project and TAPAS project; the Helmholtz Association via HI-SCORE (Helmholtz International Research School) (M.G., P.C., S.A., and D.N.); the European Union’s Horizon 2020 research and innovation program under grant agreement 763977 of the PerTPV project; the Research Council of Lithuania under grant agreement S‐MIP‐19‐5/SV3‐1079 of the SAM project (A.M. and T.M.); Slovene Research Agency (ARRS) funding through research programs P2-0197 and J2-1727 (M.J., G.M., and M.T.); Deutsche Forschungsgemeinschaft projects 423749265 and 03EE1017C-SPP 2196 (SURPRISE and HIPSTER) (M.S., D.N., and S.A.); EPSRC and D. Lidzey for Ph.D. studentship funding via CDT-PV (EP/L01551X/1) (J.A.S.); and Erasmus+ (J.A.S.). Author contributions: A.A.-A., Ei.K., B.L., and S.A. planned the experiments, coordinated the work,and prepared the figures; Er.K., A.M., and T.M. designed and synthesized the Me-4PACz SAM and the (Me-)nPACz series; A.A.-A. and B.L. processed the single-junction cells and optimized the SAM deposition; Ei.K. and B.L. processed the tandem cells; A.B.M.V. processed the Si bottom cells; A.A.-A., H.H., and J.A.M. conducted and analyzed the PL experiments; J.A.M., A.A.-A., and Ei.K. performed the EL studies. H.H. recorded the terahertz measurements and performed the data analysis; P.C., M.G., and M.S. conducted the pseudo–J-V and FF-VOC loss analysis (intensity-dependent VOC and QFLS); D.M. performed the photoelectron spectroscopy; J.A.S., D.S., and N.P. performed crystallographic analysis; G.M., M.J., B.L., and Ei.K. designed and built the tandem aging setup and recorded the long-term MPP tracks; and S.A., V.G., M.S., T.U., T.M., C.G., R.S., M.T., La.K., A.A., D.N., B.S., and B.R. supervised the projects. All authors contributed to data interpretation and manuscript writing. Competing interests: HZB and Kaunas University of Technology have filed patents for the SAM molecules described above and their use in tandem solar cells. Data and materials availability: All data are available in the main text or the supplementary materials.

Authors

Affiliations

Amran Al-Ashouri* https://orcid.org/0000-0001-5512-8034
Young Investigator Group Perovskite Tandem Solar Cells, Helmholtz-Zentrum Berlin, 12489 Berlin, Germany.
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Eike Köhnen* https://orcid.org/0000-0002-3637-4907
Young Investigator Group Perovskite Tandem Solar Cells, Helmholtz-Zentrum Berlin, 12489 Berlin, Germany.
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Bor Li https://orcid.org/0000-0003-3895-0792
Young Investigator Group Perovskite Tandem Solar Cells, Helmholtz-Zentrum Berlin, 12489 Berlin, Germany.
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Artiom Magomedov https://orcid.org/0000-0003-3159-1870
Department of Organic Chemistry, Kaunas University of Technology, Kaunas LT-50254, Lithuania.
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Hannes Hempel https://orcid.org/0000-0001-9689-9644
Department of Structure and Dynamics of Energy Materials, Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, 14109 Berlin, Germany.
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Pietro Caprioglio https://orcid.org/0000-0002-3465-2475
Young Investigator Group Perovskite Tandem Solar Cells, Helmholtz-Zentrum Berlin, 12489 Berlin, Germany.
Institute of Physics and Astronomy, University of Potsdam, 14476 Potsdam, Germany.
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José A. Márquez https://orcid.org/0000-0002-8173-2566
Department of Structure and Dynamics of Energy Materials, Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, 14109 Berlin, Germany.
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Anna Belen Morales Vilches https://orcid.org/0000-0001-8819-1312
PVcomB, Helmholtz-Zentrum Berlin, 12489 Berlin, Germany.
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Ernestas Kasparavicius
Department of Organic Chemistry, Kaunas University of Technology, Kaunas LT-50254, Lithuania.
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Joel A. Smith https://orcid.org/0000-0001-6889-4408
Young Investigator Group Active Materials and Interfaces for Stable Perovskite Solar Cells, Helmholtz-Zentrum Berlin, 12489 Berlin, Germany.
Department of Physics and Astronomy, University of Sheffield, Sheffield S3 7RH, UK.
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Nga Phung https://orcid.org/0000-0002-0328-6791
Young Investigator Group Active Materials and Interfaces for Stable Perovskite Solar Cells, Helmholtz-Zentrum Berlin, 12489 Berlin, Germany.
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Dorothee Menzel https://orcid.org/0000-0002-6303-8909
Young Investigator Group Perovskite Tandem Solar Cells, Helmholtz-Zentrum Berlin, 12489 Berlin, Germany.
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Max Grischek https://orcid.org/0000-0002-9786-4854
Young Investigator Group Perovskite Tandem Solar Cells, Helmholtz-Zentrum Berlin, 12489 Berlin, Germany.
Institute of Physics and Astronomy, University of Potsdam, 14476 Potsdam, Germany.
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Lukas Kegelmann https://orcid.org/0000-0001-8918-5096
Young Investigator Group Perovskite Tandem Solar Cells, Helmholtz-Zentrum Berlin, 12489 Berlin, Germany.
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Dieter Skroblin https://orcid.org/0000-0002-8197-2113
Physikalisch-Technische Bundesanstalt, 10587 Berlin, Germany.
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Christian Gollwitzer https://orcid.org/0000-0002-6437-8825
Physikalisch-Technische Bundesanstalt, 10587 Berlin, Germany.
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Tadas Malinauskas https://orcid.org/0000-0002-5478-6550
Department of Organic Chemistry, Kaunas University of Technology, Kaunas LT-50254, Lithuania.
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Marko Jošt https://orcid.org/0000-0003-2754-1467
Young Investigator Group Perovskite Tandem Solar Cells, Helmholtz-Zentrum Berlin, 12489 Berlin, Germany.
Faculty of Electrical Engineering, University of Ljubljana, 1000 Ljubljana, Slovenia.
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Gašper Matič https://orcid.org/0000-0001-7024-1588
Faculty of Electrical Engineering, University of Ljubljana, 1000 Ljubljana, Slovenia.
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Bernd Rech https://orcid.org/0000-0002-9718-8665
Scientific Management, Helmholtz-Zentrum Berlin, 12489 Berlin, Germany.
Faculty of Electrical Engineering and Computer Science, Technical University Berlin, 10587 Berlin, Germany.
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Rutger Schlatmann https://orcid.org/0000-0002-5951-9435
PVcomB, Helmholtz-Zentrum Berlin, 12489 Berlin, Germany.
HTW Berlin–University of Applied Sciences, 12459 Berlin, Germany.
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Marko Topič https://orcid.org/0000-0001-8089-2974
Faculty of Electrical Engineering, University of Ljubljana, 1000 Ljubljana, Slovenia.
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Lars Korte https://orcid.org/0000-0002-9207-9048
Young Investigator Group Perovskite Tandem Solar Cells, Helmholtz-Zentrum Berlin, 12489 Berlin, Germany.
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Antonio Abate https://orcid.org/0000-0002-3012-3541
Young Investigator Group Active Materials and Interfaces for Stable Perovskite Solar Cells, Helmholtz-Zentrum Berlin, 12489 Berlin, Germany.
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Bernd Stannowski https://orcid.org/0000-0003-0130-3954
PVcomB, Helmholtz-Zentrum Berlin, 12489 Berlin, Germany.
Beuth University of Applied Sciences Berlin, 13353 Berlin, Germany.
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Dieter Neher https://orcid.org/0000-0001-6618-8403
Institute of Physics and Astronomy, University of Potsdam, 14476 Potsdam, Germany.
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Martin Stolterfoht https://orcid.org/0000-0002-4023-2178
Institute of Physics and Astronomy, University of Potsdam, 14476 Potsdam, Germany.
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Thomas Unold https://orcid.org/0000-0002-5750-0693
Department of Structure and Dynamics of Energy Materials, Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, 14109 Berlin, Germany.
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Vytautas Getautis https://orcid.org/0000-0001-7695-4677
Department of Organic Chemistry, Kaunas University of Technology, Kaunas LT-50254, Lithuania.
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Steve Albrecht† https://orcid.org/0000-0001-9962-9535 [email protected]
Young Investigator Group Perovskite Tandem Solar Cells, Helmholtz-Zentrum Berlin, 12489 Berlin, Germany.
Faculty of Electrical Engineering and Computer Science, Technical University Berlin, 10587 Berlin, Germany.
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Funding Information

Deutsche Forschungsgemeinschaft: 03EE1017C - SPP 2196
Lietuvos Mokslo Taryba: S‐MIP‐19‐5/SV3‐1079
EPSRC Centre for Doctoral Training in New and Sustainable Photovoltaics: CDT-PV (EP/L01551X/1)

Notes

*
These authors contributed equally to this work.
†Corresponding author. Email: [email protected]

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