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A donor–acceptor-type hole-selective contact reducing non-radiative recombination losses in both subcells towards efficient all-perovskite tandems

Nature Energy volume 8, pages 714–724 (2023)Cite this article

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Abstract

The efficiency of all-perovskite tandem solar cells has surpassed that of single-junction perovskite solar cells, yet they still suffer from interfacial non-radiative recombination losses. Charge-selective materials that can reduce such losses as well as fabrication cost “applicable” to both subcells should be developed. Here we design a donor–acceptor-type molecule, MPA2FPh-BT-BA (2F), as a hole-selective contact suitable to both wide-bandgap (WBG) and low-bandgap (LBG) subcells for high-performance all-perovskite tandem solar cells. In the WBG cell, 2F enables efficient hole extraction and minimizes interfacial non-radiative recombination losses by passivating interfacial defects. In the LBG cell, 2F suppresses interfacial losses, regulates the crystal growth and enhances Sn–Pb perovskite film quality. As a result, 2F-treated WBG and LBG devices yield efficiencies of 19.33% (certified 19.09%) and 23.24%, respectively, enabling monolithic all-perovskite tandem solar cells with an efficiency of 27.22% (certified 26.3%) and improved operational stability.

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Fig. 1: Material properties and interconnection mechanism between ITO, hole-selective contacts and perovskites.
Fig. 2: Nearly lossless hole-selective contact in WBG perovskite and device performance.
Fig. 3: Characterization of improved LBG Sn–Pb perovskite quality and resulting device performance.
Fig. 4: PV performance of all-perovskite tandems.

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Data availability

The main data supporting the findings of this study are available within the published article and its Supplementary Information. Additional data are available from the corresponding authors on reasonable request. Source data are provided with this paper.

References

  1. Kojima, A., Teshima, K., Shirai, Y. & Miyasaka, T. Organometal halide perovskites as visible-light sensitizers for photovoltaic cells. J. Am. Chem. Soc. 131, 6050–6051 (2009).

    Google Scholar 

  2. Jeong, J. et al. Pseudo-halide anion engineering for alpha-FAPbI3 perovskite solar cells. Nature 592, 381–385 (2021).

    Google Scholar 

  3. Kim, M. et al. Conformal quantum dot-SnO2 layers as electron transporters for efficient perovskite solar cells. Science 375, 302–306 (2022).

    Google Scholar 

  4. Jiang, Q. et al. Surface reaction for efficient and stable inverted perovskite solar cells. Nature 611, 278–283 (2022).

    Google Scholar 

  5. Park, J. et al. Controlled growth of perovskite layers with volatile alkylammonium chlorides. Nature 616, 724–730 (2023).

    Google Scholar 

  6. Zhao, D. et al. Low-bandgap mixed tin–lead iodide perovskite absorbers with long carrier lifetimes for all-perovskite tandem solar cells. Nat. Energy 2, 17018 (2017).

    Google Scholar 

  7. Zhao, D. et al. Efficient two-terminal all-perovskite tandem solar cells enabled by high-quality low-bandgap absorber layers. Nat. Energy 3, 1093–1100 (2018).

    Google Scholar 

  8. Yu, Z. et al. Simplified interconnection structure based on C60/SnO2−x for all-perovskite tandem solar cells. Nat. Energy 5, 657–665 (2020).

    Google Scholar 

  9. Jiang, F. et al. A two-terminal perovskite/perovskite tandem solar cell. J. Mater. Chem. A 4, 1208–1213 (2016).

    Google Scholar 

  10. Celik, I. et al. Environmental analysis of perovskites and other relevant solar cell technologies in a tandem configuration. Energy Environ. Sci. 10, 1874–1884 (2017).

    Google Scholar 

  11. Islam, M. R. et al. Recent progress and future prospects for light management of all‐perovskite tandem solar cells. Adv. Mater. Interfaces 9, 2101144 (2022).

    Google Scholar 

  12. Zhao, D. & Ding, L. All-perovskite tandem structures shed light on thin-film photovoltaics. Sci. Bull. 65, 1144–1146 (2020).

    Google Scholar 

  13. He, R. et al. Wide-bandgap organic–inorganic hybrid and all-inorganic perovskite solar cells and their application in all-perovskite tandem solar cells. Energy Environ. Sci. 14, 5723–5759 (2021).

    Google Scholar 

  14. Tian, X., Stranks, S. D. & You, F. Life cycle energy use and environmental implications of high-performance perovskite tandem solar cells. Sci. Adv. 6, eabb0055 (2020).

    Google Scholar 

  15. Lin, R. et al. All-perovskite tandem solar cells with improved grain surface passivation. Nature 603, 73–78 (2022).

    Google Scholar 

  16. Chen, H. et al. Regulating surface potential maximizes voltage in all-perovskite tandems. Nature 613, 676–681 (2023).

    Google Scholar 

  17. Li, C. et al. Low-bandgap mixed tin-lead iodide perovskites with reduced methylammonium for simultaneous enhancement of solar cell efficiency and stability. Nat. Energy 5, 768–776 (2020).

    Google Scholar 

  18. Dai, X. et al. Efficient monolithic all-perovskite tandem solar modules with small cell-to-module derate. Nat. Energy 7, 923–931 (2022).

    Google Scholar 

  19. Wang, C. et al. A universal close-space annealing strategy towards high-quality perovskite absorbers enabling efficient all-perovskite tandem solar cells. Nat. Energy 7, 744–753 (2022).

    Google Scholar 

  20. Leijtens, T. et al. Tin-lead halide perovskites with improved thermal and air stability for efficient all-perovskite tandem solar cells. Sustain. Energy Fuels 2, 2450–2459 (2018).

    Google Scholar 

  21. Lin, R. et al. Monolithic all-perovskite tandem solar cells with 24.8% efficiency exploiting comproportionation to suppress Sn(II) oxidation in precursor ink. Nat. Energy 4, 864–873 (2019).

    Google Scholar 

  22. Tong, J. et al. Carrier lifetimes of >1 µs in Sn–Pb perovskites enable efficient all-perovskite tandem solar cells. Science 364, 475–479 (2019).

    Google Scholar 

  23. Xiao, K. et al. All-perovskite tandem solar cells with 24.2% certified efficiency and area over 1 cm2 using surface-anchoring zwitterionic antioxidant. Nat. Energy 5, 870–880 (2020).

    Google Scholar 

  24. Chen, J. & Park, N.-G. Inorganic hole-transporting materials for stable and high-efficiency perovskite solar cells. J. Phys. Chem. C 122, 14039–14063 (2018).

    Google Scholar 

  25. Jung, E. H. et al. Efficient, stable and scalable perovskite solar cells using poly(3-hexylthiophene). Nature 567, 511–515 (2019).

    Google Scholar 

  26. Al-Ashouri, A. et al. Monolithic perovskite/silicon tandem solar cell with >29% efficiency by enhanced hole extraction. Science 370, 1300–1309 (2020).

    Google Scholar 

  27. Al-Ashouri, A. et al. Conformal monolayer contacts with lossless interfaces for perovskite single junction and monolithic tandem solar cells. Energy Environ. Sci. 12, 3356–3369 (2019).

    Google Scholar 

  28. Hu, M., Bi, C., Yuan, Y., Bai, Y. & Huang, J. Stabilized wide bandgap MAPbBrxI3-x perovskite by enhanced grain size and improved crystallinity. Adv. Sci. 3, 1500301 (2016).

    Google Scholar 

  29. Stolterfoht, M. et al. Approaching the fill factor Shockley–Queisser limit in stable, dopant-free triple cation perovskite solar cells. Energy Environ. Sci. 10, 1530–1539 (2017).

    Google Scholar 

  30. Chin, Y.-C., Daboczi, M., Henderson, C., Luke, J. & Kim, J.-S. Suppressing PEDOT:PSS doping-induced interfacial recombination loss in perovskite solar cells. ACS Energy Lett. 7, 560–568 (2022).

    Google Scholar 

  31. Kapil, G. et al. Tin–lead perovskite solar cells fabricated on hole selective monolayers. ACS Energy Lett. 7, 966–974 (2022).

    Google Scholar 

  32. Chiykowski, V. A. et al. Precise control of thermal and redox properties of organic hole‐transport materials. Angew. Chem. Int. Ed. 130, 15755–15759 (2018).

    Google Scholar 

  33. Wang, Y. et al. Dopant-free small-molecule hole-transporting material for inverted perovskite solar cells with efficiency exceeding 21%. Adv. Mater. 31, 1902781 (2019).

    Google Scholar 

  34. Wang, Y. et al. Teaching an old anchoring group new tricks: enabling low-cost, eco-friendly hole-transporting materials for efficient and stable perovskite solar cells. J. Am. Chem. Soc. 142, 16632–16643 (2020).

    Google Scholar 

  35. Zhao, S. et al. Cross-plane transport in a single-molecule two-dimensional van der Waals heterojunction. Sci. Adv. 6, eaba6714 (2020).

    Google Scholar 

  36. Lin, H.-C. et al. Influence of molecular orientation on charge-transfer processes at phthalocyanine/metal oxide interfaces and relationship to organic photovoltaic performance. J. Phys. Chem. C 119, 10304–10313 (2015).

    Google Scholar 

  37. Ali, F., Roldán‐Carmona, C., Sohail, M. & Nazeeruddin, M. K. Applications of self‐assembled monolayers for perovskite solar cells interface engineering to address efficiency and stability. Adv. Energy Mater. 10, 2002989 (2020).

    Google Scholar 

  38. Caprioglio, P. et al. On the relation between the open‐circuit voltage and quasi‐Fermi level splitting in efficient perovskite solar cells. Adv. Energy Mater. 9, 1901631 (2019).

    Google Scholar 

  39. Stolterfoht, M. et al. Visualization and suppression of interfacial recombination for high-efficiency large-area pin perovskite solar cells. Nat. Energy 3, 847–854 (2018).

    Google Scholar 

  40. Stolterfoht, M. et al. How to quantify the efficiency potential of neat perovskite films: perovskite semiconductors with an implied efficiency exceeding 28%. Adv. Mater. 32, 2000080 (2020).

    Google Scholar 

  41. Li, C. et al. Reducing saturation-current density to realize high‐efficiency low‐bandgap mixed tin–lead halide perovskite solar cells. Adv. Energy Mater. 9, 1803135 (2018).

    Google Scholar 

  42. Chen, Q. et al. Unveiling roles of tin fluoride additives in high‐efficiency low‐bandgap mixed tin–lead perovskite solar cells. Adv. Energy Mater. 11, 2101045 (2021).

    Google Scholar 

  43. Wang, J. et al. Highly efficient all-inorganic perovskite solar cells with suppressed non-radiative recombination by a Lewis base. Nat. Commun. 11, 177 (2020).

    Google Scholar 

  44. Tress, W. et al. Predicting the open-circuit voltage of CH3NH3PbI3 perovskite solar cells using electroluminescence and photovoltaic quantum efficiency spectra: the role of radiative and non-radiative recombination. Adv. Energy Mater. 5, 1400812 (2015).

    Google Scholar 

  45. Zhao, Y. & Truhlar, D. G. The M06 suite of density functionals for main group thermochemistry, thermochemical kinetics, noncovalent interactions, excited states, and transition elements: two new functionals and systematic testing of four M06-class functionals and 12 other functionals. Theor. Chem. Acc. 120, 215–241 (2007).

    Google Scholar 

  46. Hay, P. J. & Wadt, W. R. Ab initio effective core potentials for molecular calculations. Potentials for K to Au including the outermost core orbitals. J. Chem. Phys. 82, 299–310 (1985).

    Google Scholar 

  47. Weigend, F. & Ahlrichs, R. Balanced basis sets of split valence, triple zeta valence and quadruple zeta valence quality for H to Rn: design and assessment of accuracy. Phys. Chem. Chem. Phys. 7, 3297–3305 (2005).

    Google Scholar 

  48. Frisch, M. J., Trucks, G. W., Schlegel, H. B., Scuseria, G. E. & Fox, D. J. Gaussian 09 Revision A.1 (Gaussian, 2009).

Download references

Acknowledgements

This work was financially supported by the National Key R&D Programme of China (number 2022YFB4200303, D.Z.), the National Natural Science Foundation of China (number 62174112, D.Z.), the Fundamental Research Funds for the Central Universities (numbers YJ201955, D.Z., YJ2021157, C.C.), the Science and Technology Programme of Sichuan Province (numbers 2020JDJQ0030, D.Z., 2020YFH0079, X.H.), the Engineering Featured Team Fund of Sichuan University (number 2020SCUNG102, D.Z.), open foundation of State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures, Guangxi University (grant number 2022GXYSOF05, C.C.) and Key Lab of Advanced Optical Manufacturing Technologies of Jiangsu Province and Key Lab of Modern Optical Technologies of Education Ministry of China, Soochow University (number KJS1909, C.W.). M.S. thanks the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation), project number 423749265 (M.S.) and 424709669-SPP 2196 (SURPRISE and HIPSTER, M.S.). M.S. further acknowledges the Heisenberg programme from the DFG for funding project number 498155101. F.F. acknowledges the funding from Swiss National Science Foundation (number 200021_213073). F.L. acknowledges the Volkswagen Foundation for support with a Freigeist Fellowship. We thank the Shiyanjia lab for the support of first-principles calculations and the molecular dynamics simulations.

Author information

Author notes

  1. These authors contributed equally: Jingwei Zhu, Yi Luo.

Authors and Affiliations

  1. College of Materials Science and Engineering & Institute of New Energy and Low-Carbon Technology & Engineering Research Center of Alternative Energy Materials and Devices, Ministry of Education, Sichuan University, Chengdu, China

    Jingwei Zhu, Yi Luo, Rui He, Cong Chen, Jincheng Luo, Zongjin Yi, Yuliang Xu, Juncheng Wang, Zhihao Zhang, Wenqing Liang, Guangyao Cui, Shengqiang Ren, Xia Hao, Lili Wu, Jingquan Zhang & Dewei Zhao

  2. Strait Institute of Flexible Electronics (SIFE, Future Technologies), Fujian Normal University and Strait Laboratory of Flexible Electronics (SLoFE), Fuzhou, China

    Yang Wang

  3. Institute of Physics and Astronomy, University of Potsdam, Potsdam, Germany

    Jarla Thiesbrummel, Felix Lang & Martin Stolterfoht

  4. Clarendon Laboratory, University of Oxford, Oxford, UK

    Jarla Thiesbrummel

  5. School of Optoelectronic Science and Engineering and Collaborative Innovation Center of Suzhou Nano Science and Technology, Key Lab of Advanced Optical Manufacturing Technologies of Jiangsu Province and Key Lab of Modern Optical Technologies of Education Ministry of China, Soochow University, Suzhou, China

    Changlei Wang

  6. Laboratory for Thin Films and Photovoltaics, Empa-Swiss Federal Laboratories for Materials Science and Technology, Duebendorf, Switzerland

    Huagui Lai & Fan Fu

  7. State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures & School of Resources, Environment and Materials, Guangxi University, Nanning, China

    Hao Huang

  8. Key Laboratory of Material Physics, Ministry of Education, School of Physics and Microelectronics, Zhengzhou University, Zhengzhou, China

    Ye Wang

  9. Key Lab of Artificial Micro- and Nano-Structures of Ministry of Education of China, School of Physics and Technology, Wuhan University, Wuhan, China

    Fang Yao & Qianqian Lin

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  1. Jingwei Zhu
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Contributions

D.Z., Yang Wang and C.C. conceived and designed the research. J. Zhu carried out the fabrication and major characterization of LBG PSCs and all-perovskite TSCs. Y.L. carried out the fabrication and major characterization of WBG PSCs. Yang Wang synthesized the SCMs and provide the relevant characterizations of SCMs. J. Zhu, Y.L., R.H., J.L., Z.Y. and Y.X. fabricated all-perovskite tandem devices. Z.Y. and J.W. helped to optimize the 1.68 eV and 1.57 eV devices. F.L., J.T. and M.S. performed the PLQY measurements of WBG PSCs. C.W. performed EQE measurements. H.L. and F.F. carried out TPV, TPC and electrochemical impedance spectroscopy measurements. F.Y. and Q.L. performed the absorption spectra of molecules and TRMC decay curves of perovskite films. J. Zhu, Yang Wang and D.Z. wrote the paper with input from all co-authors. All authors discussed the results and reviewed the paper. D.Z. directed this project.

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Correspondence to Cong Chen, Yang Wang or Dewei Zhao.

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Nature Energy thanks Antonio Facchetti and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Information

Supplementary Methods, Notes 1–4, Figs. 1–43, Tables 1–4 and References 1–19.

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Supplementary Data 1

Supplementary Figs. 18, 19a–d, 34a–d, 39c,d and 40c,d.

Source data

Source Data Fig. 4

PCE and VOC histograms of 40 tandem cells.

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Zhu, J., Luo, Y., He, R. et al. A donor–acceptor-type hole-selective contact reducing non-radiative recombination losses in both subcells towards efficient all-perovskite tandems. Nat Energy 8, 714–724 (2023). https://doi.org/10.1038/s41560-023-01274-z

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